Polycarbonate/polyorganosiloxane copolymer and resin composition including said copolymer

ABSTRACT

Provided is a polycarbonate-polyorganosiloxane copolymer, which is produced by using a diol monomer (a1) and a polyorganosiloxane (a2) satisfying the following condition, including: a polyorganosiloxane block (A-1) including a specific repeating unit; and a polycarbonate block (A-2) formed of a specific repeating unit: a mixture, which is obtained by bringing the diol monomer (a1), the polyorganosiloxane (a2), a carbonic acid diester, and a basic catalyst present at the same amount ratio as that at a time of production of the polycarbonate-polyorganosiloxane copolymer into contact with each other at from 100° C. to 250° C. for from 0.5 hour to 5 hours, has a haze value of 30 or less measured under conditions of 23° C. and an optical path length of 10 mm in conformity with ISO 14782:1999.

TECHNICAL FIELD

The present invention relates to a polycarbonate-polyorganosiloxanecopolymer and a resin composition including the copolymer.

BACKGROUND ART

A polycarbonate resin is an engineering plastic that is excellent intransparency and dynamic properties, and has extremely high impactresistance. It has been known that a polycarbonate-polyorganosiloxanecopolymer obtained by copolymerizing a polycarbonate with a polysiloxaneis excellent in low-temperature impact resistance, and is also excellentin chemical resistance while maintaining high transparency.

In general, a method including causing an aromatic dihydroxy compoundand phosgene to directly react with each other (interfacialpolycondensation method), or a method including subjecting the aromaticdihydroxy compound and a carbonic acid diester in molten states to anester exchange reaction (melt polymerization method) has been known as amethod of producing the polycarbonate resin.

An interfacial polymerization method is frequently adopted for theproduction of the polycarbonate-polyorganosiloxane copolymer. Forexample, it has been known that the copolymer can be produced asdescribed below (PTL 1). A diaryl diol compound, such as bisphenol, andphosgene are caused to react with each other in the presence of anorganic solvent to produce a polycarbonate oligomer having a reactivechloroformate group. Simultaneously or sequentially with the productionof the polycarbonate oligomer, the polycarbonate oligomer, a bisphenol,and a polysiloxane having hydroxyl group-containing aryl groups at bothterminals thereof are further brought into contact with each other in amethylene chloride/water medium to produce the copolymer. In general, ina polymerization reaction, a homocoupling body in which the molecules ofone and the same raw material component are bonded to each other may beproduced, or an unreacted raw material component may be produced becausepart of the raw materials are not involved in the polymerizationreaction. Any such component is present in a polymer to be obtained bythe reaction without being uniformly incorporated into the main chain ofthe polymer, and hence the transparency and dynamic properties of thepolymer remarkably reduce. In the interfacial polymerization method,such problem hardly occurs, and hence a polycarbonate-polyorganosiloxanecopolymer excellent in transparency and dynamic properties is obtained.

Meanwhile, in the interfacial polymerization method, phosgene havinghigh toxicity needs to be used as a carbonate source. In addition, in apolymerization reaction system, methylene chloride having a largeenvironmental load needs to be used as a solvent, and its removalrequires a large degassing apparatus and large energy, thereby leadingto an economic disadvantage. To avoid the problem, an investigation hasbeen made on the production of the polycarbonate-polyorganosiloxanecopolymer by a production method except the interfacial polymerizationmethod, such as the melt polymerization method.

In PTL 2, there is a disclosure of the production of apolycarbonate-polyorganosiloxane copolymer from a bisphenol compound, acarbonic acid aromatic diester, a silanol-terminated polysiloxane, and acatalyst by the melt polymerization method. In PTL 3, there is adisclosure of a method of producing a block copolysiloxane carbonate inthe presence of a carbonate-terminated polyorganosiloxane, a dihydroxyaromatic compound, a diaryl carbonate, and a carbonate ester exchangecatalyst. In PTL 4, there is a disclosure of a method of producing apolysiloxane/polycarbonate block co-condensation product, the methodincluding causing a hydroxyaryloxy-terminated dimethylsiloxane, and anoligocarbonate having a specific weight-average molecular weight and aspecific terminal ratio (between a OH terminal group and an arylterminal group), which are in molten states, to react with each other inthe presence of a catalyst.

In PTL 5, there is a disclosure of a method of producing apoly(diorganosiloxane)/polycarbonate block copolymer, the methodincluding subjecting a polydiorganosiloxane containing apolydiorganosiloxane component having a specific terminal structure, aSi-free diphenol, and a carbonic acid diaryl ester to meltpolymerization in the presence of a specific catalyst. In PTL 6, thereis a disclosure of a method of producing a modified polycarbonate resinthrough solid-phase polymerization, and there is a description of theuse of a polysiloxane compound as a starting raw material substance. Ineach of PTLs 7-9, there is a disclosure of a method of obtaining apolysiloxane-polycarbonate block co-condensation product through anester exchange method.

CITATION LIST Patent Literature

-   PTL 1: JP 2015-189953 A-   PTL 2: U.S. Pat. No. 5,227,449 A-   PTL 3: JP 08-311206 A-   PTL 4: JP 10-251408 A-   PTL 5: JP 2008-248262 A-   PTL 6: JP 2008-513594 T-   PTL 7: JP 2017-505841 T-   PTL 8: JP 2016-532734 T-   PTL 9: JP 2016-532733 T

SUMMARY OF INVENTION Technical Problem

In each of PTLs 2-7, there is a disclosure of the method of producing apolycarbonate-polyorganosiloxane copolymer based on the meltpolymerization method. However, the method is still insufficient interms of the production of a polycarbonate-polyorganosiloxane copolymerhaving good transparency and good dynamic properties.

In PTL 2, there is no teaching concerning the transparency of thepolymer obtained by using the silanol-terminated polysiloxane, and ithas been known that a silanol-terminated dimethylsiloxane is more liableto cause intramolecular condensation as its molecular weight reduces. Acyclic siloxane produced as a result of the intramolecular condensationremains in the polycarbonate-polyorganosiloxane copolymer to be obtainedto adversely affect the transparency and dynamic properties of thecopolymer. Moreover, concern is raised in that the cyclic siloxanecauses an adverse effect, such as a relay contact failure, inapplications in electrical and electronic fields.

In PTL 3, there is a description that the amount of apolydimethylsiloxane to be incorporated into the main chain of thepolymer increases, but there is no teaching concerning the transparencyof the polymer to be obtained. In addition, there is a description thatthe external appearances of the carbonate-terminated polyorganosiloxaneand the other raw materials in molten states are “translucent white”.Accordingly, it is assumed that the carbonate-terminatedpolyorganosiloxane is separated from the other raw materials, and hencea component produced by homocoupling and an unreactedcarbonate-terminated polyorganosiloxane still remain in the polymer.Those components remarkably reduce the transparency and dynamicproperties of the polycarbonate-polysiloxane copolymer. In PTL 3, evenin a production example in which the amount of the siloxane to beincorporated into the main chain of the polymer is large, an alkalimetal-based catalyst (sodium hydroxide) is used in an amount 10×10⁻⁶times as large as the number of moles of bisphenol A. When an excessiveamount of the catalyst is used, an increase in amount of a remainingcatalyst component induces the hydrolysis of a polycarbonate chain.Accordingly, it is assumed that the resultant polymer does not have heatresistance or weatherability enough for use under practical conditions.

The method disclosed in PTL 4 is still insufficient in terms of theuniformity of the siloxane and the other raw material at the time oftheir polymerization as can be seen from the fact that there is adescription that the external appearance of the resultant polymer is“white”. Accordingly, it can be said that the transparency and dynamicproperties of the polymer are susceptible to improvement.

The copolymer disclosed in PTL 5 has a large domain structure, and thelarge structure may adversely affect its transparency. In PTL 6, as ageneral theory, there is a description of, for example, the transparencyof a polycarbonate resin, but there is no demonstration that apolycarbonate-polyorganosiloxane copolymer has high transparency. InPTLs 7-9, the copolymers including polysiloxane blocks having the samestructure are produced by the ester exchange method (melt polymerizationmethod). However, as described in PTL 8, the resins to be obtained areeach opaque white powder.

An attempt has been made to obtain a polycarbonate-polyorganosiloxanecopolymer through an approach except the interfacial polymerizationmethod. At present, however, no effective means for obtaining apolycarbonate-polyorganosiloxane copolymer having high transparency hasbeen provided yet. An object of the present invention is to obtain apolycarbonate-polyorganosiloxane copolymer having high transparency,which is obtained by an approach except the interfacial polymerizationmethod.

Solution to Problem

The inventors of the present invention have made extensiveinvestigations, and as a result, have found that apolycarbonate-polyorganosiloxane copolymer having high transparency canbe obtained by an approach except the interfacial polymerization method.A polycarbonate-polyorganosiloxane copolymer according to one embodimentof the present invention has a specific structure.

That is, the present invention relates to the following.

[1] A polycarbonate-polyorganosiloxane copolymer, which is produced byusing a diol monomer (a1) and a polyorganosiloxane (a2) satisfying thefollowing condition, comprising: a polyorganosiloxane block (A-1)including a repeating unit represented by the following formula (1); anda polycarbonate block (A-2) formed of a repeating unit represented bythe following formula (2):

a mixture, which is obtained by bringing the diol monomer (a1), thepolyorganosiloxane (a2), a carbonic acid diester, and a basic catalystpresent at the same amount ratio as that at a time of production of thepolycarbonate-polyorganosiloxane copolymer into contact with each otherat from 100° C. to 250° C. for from 0.5 hour to 5 hours, has a hazevalue of 30 or less measured under conditions of 23° C. and an opticalpath length of 10 mm in conformity with ISO 14782:1999:

wherein R¹ and R² may be identical to or different from each other, andeach independently represent a hydrogen atom, a halogen atom, an alkylgroup having 1 to 10 carbon atoms, an alkoxy group having 1 to 10 carbonatoms, an aryl group having 6 to 12 carbon atoms, or an alkylaryl groupwhose alkyl group moiety has 1 to 10 carbon atoms, “a” represents aninteger of from 2 to 500, R¹⁰ represents a divalent aliphatichydrocarbon group having 2 to 40 carbon atoms or a divalent alicyclichydrocarbon group having 3 to 40 carbon atoms, or a divalent aromatichydrocarbon group having 6 to 20 carbon atoms, and may be substitutedwith a substituent, the divalent aliphatic hydrocarbon group, thedivalent alicyclic hydrocarbon group, or the divalent aromatichydrocarbon group may contain at least one heteroatom selected from anoxygen atom, a nitrogen atom, and a sulfur atom, or at least one halogenatom selected from a fluorine atom, a chlorine atom, a bromine atom, andan iodine atom, and “y” represents an integer of from 10 to 500.[2] The polycarbonate-polyorganosiloxane copolymer according to theabove-mentioned item [1], further comprising a structural unitrepresented by the following formula (3):

wherein R³ and R⁴ may be identical to or different from each other, andeach independently represent a hydrogen atom, a halogen atom, an alkylgroup having 1 to 10 carbon atoms, an alkoxy group having 1 to 10 carbonatoms, an aryl group having 6 to 12 carbon atoms, or an alkylaryl groupwhose alkyl group moiety has 1 to 10 carbon atoms, R⁶ represents anarylene group having 6 to 20 carbon atoms, an alkylene group having 1 to10 carbon atoms, or an alkylarylene group whose alkyl group moiety has 1to 10 carbon atoms, and may contain, as a functional group, —O—, —COO—,—CO—, —S—, —NH—, or —NR¹¹¹—, R⁸s may be identical to or different fromeach other, and each independently represent an arylene group having 6to 20 carbon atoms, an alkylene group having 1 to 10 carbon atoms, abranched alkylene group having 3 to 10 carbon atoms, or an alkylarylenegroup whose alkyl group moiety has 1 to 10 carbon atoms, and may eachcontain, as a functional group, —O—, —COO—, —CO—, —S—, —NH—, or —NR¹¹¹—,R¹¹¹ represents an alkyl group having 1 to 10 carbon atoms or an arylgroup having 6 to 10 carbon atoms, “z” represents 0 or 1, and “b”represents an integer of from 0 to 200.[3] The polycarbonate-polyorganosiloxane copolymer according to theabove-mentioned item [1] or [2], wherein the polyorganosiloxane block(A-1) includes a structure represented by the following formula (I):

wherein R¹ to R⁴ may be identical to or different from each other, andeach independently represent a hydrogen atom, a halogen atom, an alkylgroup having 1 to 10 carbon atoms, an alkoxy group having 1 to 10 carbonatoms, an aryl group having 6 to 12 carbon atoms, or an alkylaryl groupwhose alkyl group moiety has 1 to 10 carbon atoms, R⁵ and R⁶ may beidentical to or different from each other, and each independentlyrepresent an arylene group having 6 to 20 carbon atoms, an alkylenegroup having 1 to 10 carbon atoms, or an alkylarylene group whose alkylgroup moiety has 1 to 10 carbon atoms, and may each contain, as afunctional group, —O—, —COO—, —CO—, —S—, —NH—, or —NR¹¹¹—, R⁷ and R⁸ maybe identical to or different from each other, and each independentlyrepresent an arylene group having 6 to 20 carbon atoms, an alkylenegroup having 1 to 10 carbon atoms, a branched alkylene group having 3 to10 carbon atoms, or an alkylarylene group whose alkyl group moiety has 1to 10 carbon atoms, and may each contain, as a functional group, —O—,—COO—, —CO—, —S—, —NH—, or represents an alkyl group having 1 to 10carbon atoms or an aryl group having 6 to 10 carbon atoms, “z” and “z1”each independently represent 0 or 1, “a” represents an integer of from 2to 500, and “b” and “b1” each independently represent an integer of from0 to 200.[4] The polycarbonate-polyorganosiloxane copolymer according to any oneof the above-mentioned items [1] to [3], wherein the diol monomer (a1)is at least one kind of compound selected from the group consisting ofan aromatic dihydroxy compound represented by the following formula(111) and an aliphatic dihydroxy compound represented by the followingformula (112):

wherein R⁵⁵ and R⁵⁶ each independently represent a halogen atom, analkyl group having 1 to 6 carbon atoms, or an alkoxy group having 1 to 6carbon atoms, X represents a single bond, an alkylene group having 1 to8 carbon atoms, an alkylidene group having 2 to 8 carbon atoms, acycloalkylene group having 5 to 15 carbon atoms, a cycloalkylidene grouphaving 5 to 15 carbon atoms, a fluorenediyl group, an arylalkylene grouphaving 7 to 15 carbon atoms, an arylalkylidene group having 7 to 15carbon atoms, —S—, —SO—, —SO₂—, —O—, or —CO—, “s” and “t” eachindependently represent an integer of from 0 to 4, R¹⁰⁰ represents adivalent aliphatic hydrocarbon group having 2 to 40 carbon atoms, andmay include a branched structure or a cyclic structure, and R¹⁰⁰ maycontain at least one heteroatom selected from an oxygen atom, a nitrogenatom, and a sulfur atom, or at least one halogen atom selected from afluorine atom, a chlorine atom, a bromine atom, and an iodine atom.[5] The polycarbonate-polyorganosiloxane copolymer according to any oneof the above-mentioned items [1] to [4], wherein the diol monomer (a1)is an aromatic bisphenol selected from 2,2-bis(4-hydroxyphenyl)propane,2,2-bis(4-hydroxy-3-methylphenyl)propane,1,1-bis(4-hydroxyphenyl)cyclohexane,1,1-bis(4-hydroxyphenyl)-3-methylcyclohexane,1,1-bis(4-hydroxyphenyl)-3,3,5-trimethylcyclohexane, and1,1-bis(4-hydroxyphenyl)cyclododecene, or an aliphatic diol selectedfrom isosorbide, cyclohexane-1,4-dimethanol, tricyclodecanedimethanol,3,9-bis(1,1-dimethyl-2-hydroxyethyl)-2,4,8,10-tetraoxaspiro[5.5]undecane,1,3-propanediol, and 1,4-butanediol.[6] The polycarbonate-polyorganosiloxane copolymer according to any oneof the above-mentioned items [1] to [5], wherein the polycarbonate block(A-2) includes one or more selected from the group consisting ofrepeating units represented by the following formulae (a-i) to (a-v).

[7] The polycarbonate-polyorganosiloxane copolymer according to any oneof the above-mentioned items [1] to [6], wherein in the formula (1) orthe formula (I), “a” represents an integer of 2 or more and 300 or less.[8] The polycarbonate-polyorganosiloxane copolymer according to any oneof the above-mentioned items [1] to [7], wherein the polyorganosiloxaneblock (A-1) including the repeating unit represented by the formula (1)includes at least one selected from the group consisting of structuralunits represented by the following formulae (1-1) to (1-3):

wherein R¹ to R⁸, “z”, “z1”, “a”, “b”, and “b1” are as described above,and β represents a divalent group derived from a diisocyanate compound,or a divalent group derived from a dicarboxylic acid or a dicarboxylicacid halide.[9] The polycarbonate-polyorganosiloxane copolymer according to any oneof the above-mentioned items [1] to [8], wherein R¹ and R² in theformula (1), or R¹ to R⁴ in the formula (1) and the formula (3) eachrepresent a methyl group.[10] The polycarbonate-polyorganosiloxane copolymer according to any oneof the above-mentioned items [2] to [9], wherein in the formula (3), R⁶represents a trimethylene group (—(CH₂)₃—).[11] The polycarbonate-polyorganosiloxane copolymer according to any oneof the above-mentioned items [2] to [10], wherein in the formula (3), R⁸represents any structure selected from the group consisting of adimethylene group (—(CH₂)₂—), a methyl-substituted dimethylene group(—CH₂CHMe—), a trimethylene group (—(CH₂)₃—), and a tetramethylene group(—(CH₂)₄—).[12] The polycarbonate-polyorganosiloxane copolymer according to any oneof the above-mentioned items [1] to [11], wherein a content of thepolyorganosiloxane block represented by the formula (1) or the formula(I) in the polycarbonate-polyorganosiloxane copolymer is 0.1 mass % ormore and 60 mass % or less.[13] The polycarbonate-polyorganosiloxane copolymer according to any oneof the above-mentioned items [1] to [12], wherein thepolycarbonate-polyorganosiloxane copolymer has a viscosity-averagemolecular weight (Mv) of 5,000 or more and 50,000 or less.[14] The polycarbonate-polyorganosiloxane copolymer according to any oneof the above-mentioned items [1] to [13], wherein a 1-millimeter thickplate obtained by molding the polycarbonate-polyorganosiloxane copolymerhas a haze value of 40 or less measured in conformity with ISO14782:1999.[15] The polycarbonate-polyorganosiloxane copolymer according to any oneof the above-mentioned items [1] to [14], wherein thepolycarbonate-polyorganosiloxane copolymer is obtained by a meltpolymerization method.[16] The polycarbonate-polyorganosiloxane copolymer according to any oneof the above-mentioned items [1] to [15], wherein the carbonic aciddiester is at least one kind of compound selected from a diarylcarbonate compound, a dialkyl carbonate compound, and an alkyl arylcarbonate compound.[17] The polycarbonate-polyorganosiloxane copolymer according to any oneof the above-mentioned items [1] to [16], wherein the basic catalyst isat least one kind selected from the group consisting of an alkali metalcompound, an alkaline earth metal compound, a nitrogen-containingcompound, a quaternary phosphonium salt containing an aryl group, and ametal compound.[18] A polycarbonate-based resin composition, comprising thepolycarbonate-polyorganosiloxane copolymer of any one of theabove-mentioned items [1] to [17].[19] The polycarbonate-based resin composition according to theabove-mentioned item [18], further comprising an inorganic filler.[20] The polycarbonate-based resin composition according to theabove-mentioned item [19], wherein the polycarbonate-based resincomposition comprises 1 part by mass to 150 parts by mass of theinorganic filler with respect to 100 parts by mass of thepolycarbonate-polyorganosiloxane copolymer.[21] The polycarbonate-based resin composition according to theabove-mentioned item [19] or [20], wherein the inorganic filler is aglass fiber or a carbon fiber.[22] A molded body, comprising the polycarbonate-based resin compositionof any one of the above-mentioned items [18] to [21].

Advantageous Effects of Invention

According to the present invention, the polycarbonate-polyorganosiloxanecopolymer having high transparency can be obtained by an approach exceptthe interfacial polymerization method.

DESCRIPTION OF EMBODIMENTS

A polycarbonate-polyorganosiloxane copolymer and a polycarbonate-basedresin composition including the copolymer of the present invention aredescribed in detail below. Herein, a specification considered to bepreferred may be arbitrarily adopted, and a combination of preferredspecifications can be said to be more preferred. The term “XX to YY” asused herein means “XX or more and YY or less.”

<Polycarbonate-Polyorganosiloxane Copolymer>

The polycarbonate-polyorganosiloxane copolymer of the present inventioncomprises a polyorganosiloxane block (A-1) including a repeating unitrepresented by the following formula (1) and a polycarbonate block (A-2)formed of a repeating unit represented by the following formula (2), andis produced by using a diol monomer (a1) and a polyorganosiloxane (a2)satisfying the following condition:

a mixture, which is obtained by bringing the diol monomer (a1), thepolyorganosiloxane (a2), a carbonic acid diester, and a basic catalystinto contact with each other at from 100° C. to 250° C. for from 0.5hour to 5 hours, has a haze value of 30 or less measured underconditions of 23° C. and an optical path length of 10 mm in conformitywith ISO 14782:1999:

wherein R¹ and R² may be identical to or different from each other, andeach independently represent a hydrogen atom, a halogen atom, an alkylgroup having 1 to 10 carbon atoms, an alkoxy group having 1 to 10 carbonatoms, an aryl group having 6 to 12 carbon atoms, or an alkylaryl groupwhose alkyl group moiety has 1 to 10 carbon atoms, “a” represents aninteger of from 2 to 500, R¹⁰ represents a divalent aliphatichydrocarbon group having 2 to 40 carbon atoms or a divalent alicyclichydrocarbon group having 3 to 40 carbon atoms, or a divalent aromatichydrocarbon group having 6 to 20 carbon atoms, and may be substitutedwith a substituent, the divalent aliphatic hydrocarbon group, thedivalent alicyclic hydrocarbon group, or the divalent aromatichydrocarbon group may contain at least one heteroatom selected from anoxygen atom, a nitrogen atom, and a sulfur atom, or at least one halogenatom selected from a fluorine atom, a chlorine atom, a bromine atom, andan iodine atom, and “y” represents an integer of from 10 to 500.

The haze value is a value obtained by subjecting a glass cell having anoptical path length of 10 mm, which is filled with the mixture, tomeasurement with a haze-measuring apparatus at 23° C. in conformity withISO 14782:1999.

The inventors of the present invention have found that when the hazevalue of the mixture of the raw materials for thepolycarbonate-polyorganosiloxane copolymer after its heating treatmentdeviates from the above-mentioned range, the transparency of thepolycarbonate-polyorganosiloxane copolymer to be obtained reduces. Theinventors have found that when such diol monomer and polyorganosiloxanethat the haze value of the raw material mixture after the heatingtreatment becomes 30 or less are used as raw materials in the presentinvention, a polycarbonate-polyorganosiloxane copolymer having hightransparency is finally obtained.

That is, the raw materials at the time of the production of thepolycarbonate-polyorganosiloxane copolymer are obtained, and then partof the raw materials are collected to provide the above-mentionedmixture, followed by the measurement of the haze value of the mixture.When the haze value of the measurement mixture satisfies theabove-mentioned requirement, the polycarbonate-polyorganosiloxanecopolymer is produced by using the raw materials. Thepolycarbonate-polyorganosiloxane copolymer to be obtained has hightransparency.

When the haze value of the raw material mixture measured under theabove-mentioned conditions becomes 30 or less, in other words, when rawmaterials that are highly compatible with each other are used, thepolymerization becomes a uniform system. It is assumed that as a resultof the foregoing, the reaction ratio of the polyorganosiloxane wasimproved to express such an effect that the polyorganosiloxane wasincorporated into the polycarbonate-polyorganosiloxane copolymer withhigh randomness, and hence the transparency of thepolycarbonate-polyorganosiloxane copolymer to be obtained was improved.

The desired haze value of the raw material mixture is obtained by, forexample, introducing a substituent having a repeating chain structurecontaining a polar functional group, which is a substituent having ahigh affinity for a hydroxyl group of the diol monomer, into a terminalof the polyorganosiloxane.

The above-mentioned substituent having a repeating chain structure canbe brought into contact with a larger number of molecules of the diolmonomer than a substituent free of any repeating chain structure does,and is hence assumed to be capable of being strongly compatible with thediol monomer. Accordingly, it is assumed that in the case where thesubstituent having a repeating chain structure is introduced into theterminal of the polyorganosiloxane, an affinity between thepolyorganosiloxane and the diol monomer can be improved as compared tothe case where the substituent having a repeating chain structure is notintroduced into the terminal.

The haze value of the mixture, which is obtained by bringing the diolmonomer (a1), the polyorganosiloxane (a2), the carbonic acid diester,and the basic catalyst into contact with each other at from 100° C. to250° C. for from 0.5 hour to 5 hours, measured under the conditions of23° C. and an optical path length of 10 mm, the haze value being acondition to be satisfied by the polycarbonate-polyorganosiloxanecopolymer of the present invention, is preferably 20 or less, morepreferably 10 or less, still more preferably 5 or less, still morepreferably 1 or less.

The mixture for measuring the haze value needs to be obtained bybringing the raw materials into contact with each other at from 100° C.to 250° C. for from 0.5 hour to 5 hours. The temperature condition forobtaining the mixture is preferably from 150° C. to 250° C., morepreferably from 180° C. to 250° C., and the contact time for obtainingthe mixture is preferably from 0.7 hour to 4 hours, more preferably from0.7 hour to 2 hours. When the temperature condition and the contact timefor obtaining the mixture fall within the ranges, and the mixtureobtained under the conditions has the haze value specified in thepresent invention, a polycarbonate-polyorganosiloxane copolymer havinghigher transparency can be obtained.

<Diol Monomer (a1)>

The diol monomer (a1) is not particularly limited as long as the monomerhas a structure represented by the following formula (a1). An aromaticdihydroxy compound or an aliphatic dihydroxy compound may be used as thediol monomer (a1).

HO—R¹⁰—OH  (a1)

In the formula (a1), 10° represents a divalent aliphatic hydrocarbongroup having 2 to 40 carbon atoms or a divalent alicyclic hydrocarbongroup having 3 to 40 carbon atoms, or a divalent aromatic hydrocarbongroup having 6 to 20 carbon atoms, and may be substituted with asubstituent, and the divalent aliphatic hydrocarbon group, the divalentalicyclic hydrocarbon group, or the divalent aromatic hydrocarbon groupmay contain at least one heteroatom selected from an oxygen atom, anitrogen atom, and a sulfur atom, or at least one halogen atom selectedfrom a fluorine atom, a chlorine atom, a bromine atom, and an iodineatom.

Examples of the divalent aliphatic hydrocarbon group having 2 to 40carbon atoms include an ethylene group, a n-propylene group, anisopropylene group, a n-butylene group, an isobutylene group, an-pentylene group, a n-hexylene group, a n-heptylene group, a n-octylenegroup, a 2-ethylhexylene group, a n-nonylene group, a n-decylene group,a n-undecylene group, a n-dodecylene group, a n-tridecylene group, an-tetradecylene group, a n-pentadecylene group, a n-hexadecylene group,a n-heptadecylene group, and a n-octadecylene group. Examples of thedivalent alicyclic hydrocarbon group having 3 to 40 carbon atoms includea cyclopentylene group, a cyclohexylene group, a cyclooctylene group, acyclodecylene group, a cyclotetradecylene group, an adamantylene group,a bicycloheptylene group, a bicyclodecylene group, and atricyclodecylene group.

As the divalent aromatic hydrocarbon group having 6 to 20 carbon atoms,there may be given various groups, and in particular, examples thereofmay include divalent aromatic hydrocarbon groups derived from, forexample, 2,2-bis(4-hydroxyphenyl)propane [bisphenol A],bis(4-hydroxyphenyl)methane, 1,1-bis(4-hydroxyphenyl)ethane,2,2-bis(4-hydroxy-3,5-dimethylphenyl)propane, 4,4′-dihydroxydiphenyl, abis(4-hydroxyphenyl)cycloalkane, bis(4-hydroxyphenyl) oxide,bis(4-hydroxyphenyl) sulfide, bis(4-hydroxyphenyl) sulfone,bis(4-hydroxyphenyl) sulfoxide, and bis(4-hydroxyphenyl) ketone.Examples thereof may also include divalent aromatic hydrocarbon groupsderived from, for example, hydroquinone, resorcin, and catechol. Thosedivalent aromatic hydrocarbon groups may be used alone or in combinationthereof.

The diol monomer (a1) may be specifically, for example, at least onekind of compound selected from the group consisting of an aromaticdihydroxy compound represented by the following formula (111) and analiphatic dihydroxy compound represented by the following formula (112):

wherein R⁵⁵ and R⁵⁶ each independently represent a halogen atom, analkyl group having 1 to 6 carbon atoms, or an alkoxy group having 1 to 6carbon atoms, X represents a single bond, an alkylene group having 1 to8 carbon atoms, an alkylidene group having 2 to 8 carbon atoms, acycloalkylene group having 5 to 15 carbon atoms, a cycloalkylidene grouphaving 5 to 15 carbon atoms, a fluorenediyl group, an arylalkylene grouphaving 7 to 15 carbon atoms, an arylalkylidene group having 7 to 15carbon atoms, —S—, —SO—, —SO₂—, —O—, or —CO—, “s” and “t” eachindependently represent an integer of from 0 to 4, R¹⁰⁰ represents adivalent aliphatic hydrocarbon group having 2 to 40 carbon atoms, andmay include a branched structure or a cyclic structure, and R¹⁰⁰ maycontain at least one heteroatom selected from an oxygen atom, a nitrogenatom, and a sulfur atom, or at least one halogen atom selected from afluorine atom, a chlorine atom, a bromine atom, and an iodine atom.

The aromatic dihydroxy compound represented by the formula (111) isdescribed in detail. Examples of the halogen atom that R⁵⁵ and R⁵⁶ inthe formula (111) each independently represent include a fluorine atom,a chlorine atom, a bromine atom, and an iodine atom.

Examples of the alkyl group that R⁵⁵ and R⁵⁶ each independentlyrepresent include a methyl group, an ethyl group, a n-propyl group, anisopropyl group, various butyl groups (the term “various” means that alinear group and various branched groups are included, and the sameapplies to the following), various pentyl groups, and various hexylgroups. Examples of the alkoxy group that R⁵⁵ and R⁵⁶ each independentlyrepresent include alkoxy groups whose alkyl group moieties are theabove-mentioned alkyl groups.

Examples of the alkylene group represented by X include a methylenegroup, an ethylene group, a trimethylene group, a tetramethylene group,and a hexamethylene group. Among them, an alkylene group having 1 to 5carbon atoms is preferred. Examples of the alkylidene group representedby X include an ethylidene group and an isopropylidene group. Examplesof the cycloalkylene group represented by X include a cyclopentanediylgroup, a cyclohexanediyl group, and a cyclooctanediyl group. Among them,a cycloalkylene group having 5 to 10 carbon atoms is preferred. Examplesof the arylene group represented by X include a phenylene group, anaphthylene group, and a biphenylene group. Examples of thecycloalkylidene group represented by X include a cyclohexylidene group,a 3,5,5-trimethylcyclohexylidene group, and a 2-adamantylidene group.Among them, a cycloalkylidene group having 5 to 10 carbon atoms ispreferred, and a cycloalkylidene group having 5 to 8 carbon atoms ismore preferred. Examples of the aryl moiety of the arylalkylene grouprepresented by X include aryl groups each having 6 to 14 ring-formingcarbon atoms, such as a phenyl group, a naphthyl group, a biphenylgroup, and an anthryl group. Examples of the aryl moiety of thearylalkylidene group represented by X include aryl groups each having 6to 14 ring-forming carbon atoms, such as a phenyl group, a naphthylgroup, a biphenyl group, and an anthryl group.

“s” and “t” each independently represent an integer of from 0 to 4,preferably from 0 to 2, more preferably 0 or 1. Among them, a compoundin which “s” and “t” each represent 0, and X represents a single bond oran alkylene group having 1 to 8 carbon atoms, or a compound in which “s”and “t” each represent 0, and X represents an alkylidene group, inparticular, an isopropylidene group is suitable.

The aliphatic dihydroxy compound represented by the formula (112) isdescribed in detail.

The divalent aliphatic hydrocarbon group having 2 to 40 carbon atomsthat is represented by R¹⁰⁰ is specifically an alkylene group havingpreferably 2 to 18, more preferably 2 to 10, still more preferably 3 to6 carbon atoms, a cycloalkylene group having preferably 4 to 20, morepreferably 5 to 20 carbon atoms, or a divalent oxygen- ornitrogen-containing saturated heterocyclic group having preferably 4 to20, more preferably 5 to 20 carbon atoms.

Examples of the alkylene group having 2 to 18 carbon atoms include anethylene group, a n-propylene group, an isopropylene group, a n-butylenegroup, an isobutylene group, a n-pentylene group, a n-hexylene group, an-heptylene group, a n-octylene group, a 2-ethylhexylene group, an-nonylene group, a n-decylene group, a n-undecylene group, an-dodecylene group, a n-tridecylene group, a n-tetradecylene group, an-pentadecylene group, a n-hexadecylene group, a n-heptadecylene group,and a n-octadecylene group. Examples of the cycloalkylene group having 4to 20 carbon atoms include a cyclopentylene group, a cyclohexylenegroup, a cyclooctylene group, a cyclodecylene group, acyclotetradecylene group, an adamantylene group, a bicycloheptylenegroup, a bicyclodecylene group, and a tricyclodecylene group. Examplesof the divalent oxygen- or nitrogen-containing saturated heterocyclicgroup may include groups each containing an oxygen or nitrogen atom inthe skeleton of any one of the above-mentioned cycloalkylene groups.

Examples of the aliphatic dihydroxy compound include: dihydroxycompounds each having a chain aliphatic hydrocarbon group, such asethylene glycol, 1,3-propanediol, 1,2-propanediol, 1,4-butanediol,1,5-pentanediol, 1,6-hexanediol, 1,7-heptanediol, 1,8-octanediol,1,10-decanediol, 2,2-dimethylpropane-1,3-diol, diethylene glycol,triethylene glycol, tetraethylene glycol, octaethylene glycol,dipropylene glycol, N-methyldiethanolamine, and p-xylylene glycol;dihydroxy compounds each having an alicyclic hydrocarbon group, such as1,2-cyclohexanediol, 1,3-cyclohexanediol, 1,4-cyclohexanediol,1,2-cyclohexanedimethanol, 1,3-cyclohexanedimethanol,1,4-cyclohexanedimethanol, 2,6-decalindiol, 1,5-decalindiol,2,3-decalindiol, 2,6-decalindimethanol, 1,5-decalindimethanol,2,3-decalindimethanol, 2,3-norbornanediol, 2,5-norbornanediol,2,3-norbornanedimethanol, 2,5-norbornanedimethanol,2,2-bis(4-hydroxycyclohexyl)-propane, 1,3-adamantanediol,1,3-adamantanedimethanol, and tricyclodecanedimethanol; condensedpolycyclic ether diols, such as isosorbide; heterocyclic spirocompounds, such as3,9-bis(2-hydroxyethyl)-2,4,8,10-tetraoxaspiro[5.5]undecane,3,9-bis(2-hydroxy-1,1-dimethylethyl)-2,4,8,10-tetraoxaspiro[5.5]undecane,3,9-bis(2-hydroxy-1,1-diethylethyl)-2,4,8,10-tetraoxaspiro[5.5]undecane,3,9-bis(2-hydroxy-1,1-dipropylethyl)-2,4,8,10-tetraoxaspiro[5.5]undecane,and a cyclic ether diol, such as 1,4-anhydroerythritol; cyclic acetaldiols, such as2-(5-ethyl-5-hydroxymethyl-1,3-dioxan-2-yl)-2-methylpropan-1-ol;N-heterocyclic diols, such as 3,4-pyrrolidinediol,3,4-dimethylpiperidinediol, N-ethyl-3,4-piperidinediol, andN-ethyl-3,5-piperidinediol; and S-heterocyclic diols, such asdeoxythiofructose.

Specifically, the aliphatic dihydroxy compound may be particularlypreferably, for example, an aliphatic diol selected from isosorbide,cyclohexane-1,4-dimethanol, tricyclodecanedimethanol,3,9-bis(2-hydroxy-1,1-dimethylethyl)-2,4,8,10-tetraoxaspiro[5.5]undecane,1,3-propanediol, and 1,4-butanediol.

The aromatic dihydroxy compound may be, for example, an aromaticbisphenol compound. The compound may be particularly preferably, forexample, an aromatic bisphenol selected from compounds represented bythe following formulae.

Specifically, bisphenol A (2,2-bis(4-hydroxyphenyl)propane), bisphenol C(2,2-bis(4-hydroxy-3-methylphenyl)propane), bisphenol Z(1,1-bis(4-hydroxyphenyl)cyclohexane), bisphenol 3MZ(1,1-bis(4-hydroxyphenyl)-3-methylcyclohexane), bisphenol HTG(1,1-bis(4-hydroxyphenyl)-3,3,5-trimethylcyclohexane), or bisphenol-CDE(1,1-bis(4-hydroxyphenyl)cyclododecene) is more preferably used.

Among them, the aliphatic diol is preferably used as the diol monomer(a1) because the haze value of the mixture, which is obtained bybringing the diol monomer (a1), the polyorganosiloxane (a2), thecarbonic acid ester compound, and the basic catalyst into contact witheach other at from 100° C. to 250° C. for from 0.5 hour to 5 hours,measured under the conditions of 23° C. and an optical path length of 10mm in conformity with ISO 14782:1999 reduces, and the total lighttransmittance of the polycarbonate-polyorganosiloxane copolymer to befinally obtained increases.

<Polyorganosiloxane (a2)>

The polyorganosiloxane (a2) preferably has a structure represented bythe following formula (a2-0):

wherein R′ to R⁴ may be identical to or different from each other, andeach independently represent a hydrogen atom, a halogen atom, an alkylgroup having 1 to 10 carbon atoms, an alkoxy group having 1 to 10 carbonatoms, an aryl group having 6 to 12 carbon atoms, or an alkylaryl groupwhose alkyl group moiety has 1 to 10 carbon atoms, R⁵ and R⁶ may beidentical to or different from each other, and each independentlyrepresent an arylene group having 6 to 20 carbon atoms, an alkylenegroup having 1 to 10 carbon atoms, or an alkylarylene group whose alkylgroup moiety has 1 to 10 carbon atoms, and may each contain, as afunctional group, —O—, —COO—, —CO—, —S—, —NH—, or —NR¹¹¹—, R¹¹¹represents an alkyl group having 1 to 10 carbon atoms or an aryl grouphaving 6 to 10 carbon atoms, and “a” represents an integer of from 2 to500.

R^(40′) represents a divalent aliphatic hydrocarbon group having 2 to380 carbon atoms, a divalent alicyclic hydrocarbon group having 3 to 380carbon atoms, or a divalent aromatic hydrocarbon group having 6 to 380carbon atoms, and may be substituted with a substituent, the divalentaliphatic hydrocarbon group, the divalent alicyclic hydrocarbon group,or the divalent aromatic hydrocarbon group may contain at least oneheteroatom selected from an oxygen atom, a nitrogen atom, and a sulfuratom, or at least one halogen atom selected from a fluorine atom, achlorine atom, a bromine atom, and an iodine atom, R^(40″) represents adivalent aliphatic hydrocarbon group having 1 to 20 carbon atoms, adivalent alicyclic hydrocarbon group having 3 to 20 carbon atoms, or adivalent aromatic hydrocarbon group having 6 to 20 carbon atoms, and maybe substituted with a substituent, and “e” and “u” each represent 0 or1.

When R⁵ and R⁶ each represent an alkylene group, its number of carbonatoms is preferably from 1 to 5.

The polyorganosiloxane preferably includes, as R^(40′), a repeatingchain structure in which at least two structures each containing atleast one hydrocarbon group selected from a divalent aliphatichydrocarbon group having 1 to 20 carbon atoms, a divalent alicyclichydrocarbon group having 3 to 20 carbon atoms, and a divalent aromatichydrocarbon group having 6 to 20 carbon atoms, and each containing atleast one heteroatom selected from the group consisting of an oxygenatom, a nitrogen atom, and a sulfur atom are linked to each other. Thestructure containing at least one hydrocarbon group selected from adivalent aliphatic hydrocarbon group having 1 to 20 carbon atoms, adivalent alicyclic hydrocarbon group having 3 to 20 carbon atoms, and adivalent aromatic hydrocarbon group having 6 to 20 carbon atoms, andcontaining at least one heteroatom selected from the group consisting ofan oxygen atom, a nitrogen atom, and a sulfur atom is preferably astructure containing at least one structure selected from the groupconsisting of —OH, —O—, —(C═O)—, —O(C═O)—, —O(C═O)O—, —NH₂, —NRH, —NR—,—NR—(C═O)—, —N═CR—, —SH, —S—, —S—S—, and —(S═O)—. R represents ahydrogen atom, a monovalent aliphatic hydrocarbon group having 1 to 20carbon atoms, or a monovalent aromatic hydrocarbon group having 6 to 20carbon atoms, and the hydrocarbon groups may each be substituted with asubstituent. Preferred examples of the repeating chain structure mayinclude the following structures: polyether, polyacetal, polylactone,polyacrylate, polyester, polycarbonate, polyketone, polysulfide,polysulfone, polyamide, and polyimide.

Among them, at least one selected from the group consisting ofpolyether, polyacrylate, and polycarbonate is preferred, and polyetheris most preferred. As the polyether, a polyalkylene ether is preferred.Among them, polyethylene glycol, polypropylene glycol, polytrimethyleneglycol, and polytetramethylene glycol are preferred. The above-mentionedstructures are preferred from the viewpoint of improving the affinity ofthe polyorganosiloxane for the diol monomer (a1) to perform uniformpolymerization.

The polyorganosiloxane (a2) more preferably has a structure representedby any one of the following formulae (a2-1) to (a2-3):

wherein R¹ to R⁴ may be identical to or different from each other, andeach independently represent a hydrogen atom, a halogen atom, an alkylgroup having 1 to 10 carbon atoms, an alkoxy group having 1 to 10 carbonatoms, an aryl group having 6 to 12 carbon atoms, or an alkylaryl groupwhose alkyl group moiety has 1 to 10 carbon atoms, R⁵ and R⁶ may beidentical to or different from each other, and each independentlyrepresent an arylene group having 6 to 20 carbon atoms, an alkylenegroup having 1 to 10 carbon atoms, or an alkylarylene group whose alkylgroup moiety has 1 to 10 carbon atoms, and may each contain, as afunctional group, —O—, —COO—, —CO—, —S—, —NH—, or —NR¹¹¹—, R⁷ and R⁸ maybe identical to or different from each other, and each independentlyrepresent an arylene group having 6 to 20 carbon atoms, an alkylenegroup having 1 to 10 carbon atoms, a branched alkylene group having 3 to10 carbon atoms, or an alkylarylene group whose alkyl group moiety has 1to 10 carbon atoms, and may each contain, as a functional group, —O—,—COO—, —CO—, —S—, —NH—, or —NR¹¹¹—, R¹¹¹ represents an alkyl grouphaving 1 to 10 carbon atoms or an aryl group having 6 to 10 carbonatoms, β represents a divalent group derived from a diisocyanatecompound, or a divalent group derived from a dicarboxylic acid or adicarboxylic acid halide, “z” and “z1” each independently represent 0 or1, “a” represents an integer of from 2 to 500, and “b” and “b1” eachindependently represent an integer of from 0 to 200.

The above-mentioned structures are preferred from the viewpoint ofimproving the affinity of the polyorganosiloxane for the diol monomer(a1) to perform uniform polymerization.

Examples of the halogen atom represented by any one of R¹ to R⁴ in theformulae (a2-0) and (a2-1) to (a2-3) include a fluorine atom, a chlorineatom, a bromine atom, and an iodine atom. Examples of the alkyl grouphaving 1 to 10 carbon atoms that is represented by any one of R¹ to R⁴include a methyl group, an ethyl group, a n-propyl group, an isopropylgroup, various butyl groups, various pentyl groups, and various hexylgroups. Examples of the alkoxy group represented by any one of R¹ to R⁴include alkoxy groups whose alkyl group moieties are the above-mentionedalkyl groups. Examples of the aryl group represented by any one of R¹ toR⁴ include a phenyl group and a naphthyl group. Examples of thealkylaryl group represented by any one of R¹ to R⁴ include alkylarylgroups whose alkyl group moieties are the above-mentioned alkyl groupsand whose aryl group moieties are the above-mentioned aryl groups.

R¹ to R⁴ each preferably represent a hydrogen atom, an alkyl grouphaving 1 to 6 carbon atoms, an alkoxy group having 1 to 6 carbon atoms,an aryl group having 6 to 12 carbon atoms, or an alkylaryl group having1 to 10 carbon atoms, and each more preferably represent a methyl group.

Examples of the arylene group having 6 to 20 carbon atoms that isrepresented by any one of R⁵ and R⁶ in the formulae (a2-0) and (a2-1) to(a2-3) include a phenylene group and a naphthylene group. Examples ofthe alkylene group having 1 to 10 carbon atoms that is represented byany one of R⁵ and R⁶ include a methylene group, a dimethylene group, atrimethylene group, a methyl-substituted dimethylene group, and atetramethylene group (the tetramethylene group may have a branchedstructure). Examples of the alkylarylene group that is represented byany one of R⁵ and R⁶ include alkylarylene groups whose alkyl groupmoieties are the above-mentioned alkyl groups and whose arylene groupmoieties are the above-mentioned arylene groups.

Each of R⁵ and R⁶ preferably represents an alkylene group having 1 to 10carbon atoms, and more preferably represents a dimethylene group, amethyl-substituted dimethylene group, or a trimethylene group. It isparticularly preferred that R⁶ in each of the formulae represent atrimethylene group (—(CH₂)₃—).

Examples of the arylene group having 6 to 20 carbon atoms that isrepresented by any one of R⁷ and R⁸ in the formulae (a2-1) to (a2-3)include a phenylene group and a naphthylene group. Examples of thealkylene group having 1 to 10 carbon atoms that is represented by anyone of R⁷ and R⁸ in the formulae (a2-1) to (a2-3) include a methylenegroup, a dimethylene group, a trimethylene group, a methyl-substituteddimethylene group, and a tetramethylene group (the tetramethylene groupmay have a branched structure). Examples of the alkylarylene grouprepresented by any one of R⁷ and R⁸ in the formulae (a2-1) to (a2-3)include alkylarylene groups whose alkyl group moieties are theabove-mentioned alkyl groups and whose arylene group moieties are theabove-mentioned arylene groups.

Each of R⁷ and R⁸ in the formulae (a2-1) to (a2-3) preferably representsan alkylene group having 1 to 10 carbon atoms, and more preferablyrepresents any structure selected from the group consisting of adimethylene group (—(CH₂)₂—), a methyl-substituted dimethylene group(—CH₂CHMe—), a trimethylene group (—(CH₂)₃—), and a tetramethylene group(—(CH₂)₄—). The above-mentioned structures are preferred from theviewpoint of improving the affinity of the polyorganosiloxane for thediol monomer (a1) to perform uniform polymerization.

A polyorganosiloxane represented by any one of the formulae (a2-1) to(a2-3) in which R¹ to R⁴ each represent a methyl group, R⁵ and R⁶ eachrepresent a trimethylene group, and R⁷ and R⁸ each represent an ethylgroup is particularly preferred.

β represents a divalent group derived from a diisocyanate compound, or adivalent group derived from a dicarboxylic acid or a dicarboxylic acidhalide, and examples thereof include divalent groups represented by thefollowing formulae (iii) to (vii):

wherein

in the formulae (a2-0) and (a2-1) to (a2-3), “a” represents the chainlength of the polyorganosiloxane, and represents an integer of 2 or moreand 500 or less, preferably 2 or more and 300 or less, more preferably10 or more and 100 or less, still more preferably 15 or more and 70 orless, still more preferably 20 or more and 65 or less. “a” preferablyfalls within the ranges because the polycarbonate-polyorganosiloxanecopolymer has a higher total light transmittance, and hence serves as ahighly transparent copolymer. The above-mentioned structures arepreferred from the viewpoint of improving the affinity of thepolyorganosiloxane for the diol monomer (a1) to perform uniformpolymerization.

In the formulae (a2-1) to (a2-3), “b” and “b1” each independentlyrepresent an integer of 0 or more and 200 or less, preferably 2 or moreand 100 or less, more preferably 5 or more and 50 or less, still morepreferably 8 or more and 25 or less. “b” and “b1” each preferably fallwithin the ranges because of the ease of availability of a raw materialfor the polyorganosiloxane. “b” and “b1” each more preferably represent100 or less because a reduction in handleability of thepolyorganosiloxane due to an increase in viscosity or melting pointthereof can be suppressed, and “b” and “b1” each still more preferablyrepresent 50 or less because the content of the polyorganosiloxane blockin the resin can be kept at such an amount that a physicalproperty-improving effect can be maintained.

In each of the formulae (a2-1) to (a2-3), “z” and “z1” eachindependently represent 0 or 1, preferably 0.

The polycarbonate-polyorganosiloxane copolymer of the present inventionincludes the polyorganosiloxane block (A-1) including the repeating unitrepresented by the following formula (1) and the polycarbonate block(A-2) formed of the repeating unit represented by the following formula(2):

wherein R¹ and R², R¹⁰, “a”, and “y” are as described above.

In the polycarbonate-polyorganosiloxane copolymer of the presentinvention, the polyorganosiloxane block (A-1) including the repeatingunit represented by the formula (1) preferably has a structurerepresented by the following formula (1A). In this case, thesilicon-side bond of the structure represented by the formula (1A) isbonded to the oxygen of the polyorganosiloxane block represented by theformula (1).

wherein

in the formula (1A), R¹ to R⁴, R⁶, and “a” are as described above,

R^(40′) represents a divalent aliphatic hydrocarbon group having 2 to380 carbon atoms, a divalent alicyclic hydrocarbon group having 3 to 380carbon atoms, or a divalent aromatic hydrocarbon group having 6 to 380carbon atoms, and may be substituted with a substituent, the divalentaliphatic hydrocarbon group, the divalent alicyclic hydrocarbon group,or the divalent aromatic hydrocarbon group may contain at least oneheteroatom selected from an oxygen atom, a nitrogen atom, and a sulfuratom, or at least one halogen atom selected from a fluorine atom, achlorine atom, a bromine atom, and an iodine atom, R⁴⁰″ represents adivalent aliphatic hydrocarbon group having 1 to 20 carbon atoms, adivalent alicyclic hydrocarbon group having 3 to 20 carbon atoms, or adivalent aromatic hydrocarbon group having 6 to 20 carbon atoms, and maybe substituted with a substituent, and “e” and “u” each represent 0 or1.

The structure preferably includes, as R^(40′), a repeating chainstructure in which at least two structures each containing at least onehydrocarbon group selected from a divalent aliphatic hydrocarbon grouphaving 1 to 20 carbon atoms, a divalent alicyclic hydrocarbon grouphaving 3 to 20 carbon atoms, and a divalent aromatic hydrocarbon grouphaving 6 to 20 carbon atoms, and each containing at least one heteroatomselected from the group consisting of an oxygen atom, a nitrogen atom,and a sulfur atom are linked to each other. Preferred examples of therepeating chain structure may include the following structures:polyether, polyacetal, polylactone, polyacrylate, polyester,polycarbonate, polyketone, polysulfide, poly sulfone, polyamide, andpolyimide.

Among them, at least one selected from the group consisting ofpolyether, polyacrylate, and polycarbonate is preferred, and polyetheris most preferred. As the polyether, polyalkylene ethers are preferred.Among them, polyethylene glycol, polypropylene glycol, polytrimethyleneglycol, and polytetramethylene glycol are preferred.

The polycarbonate-polyorganosiloxane copolymer of the present inventionmore preferably includes a structure represented by the followingformula (3). In this case, the silicon-side bond of the structurerepresented by the formula (3) is bonded to the oxygen of thepolyorganosiloxane block represented by the formula (1):

wherein R³ and R⁴ may be identical to or different from each other, andeach independently represent a hydrogen atom, a halogen atom, an alkylgroup having 1 to 10 carbon atoms, an alkoxy group having 1 to 10 carbonatoms, an aryl group having 6 to 12 carbon atoms, or an alkylaryl groupwhose alkyl group moiety has 1 to 10 carbon atoms, R⁶ represents anarylene group having 6 to 20 carbon atoms, an alkylene group having 1 to10 carbon atoms, or an alkylarylene group whose alkyl group moiety has 1to 10 carbon atoms, and may contain, as a functional group, —O—, —COO—,—CO—, —S—, —NH—, or —NR¹¹¹—, R⁸s may be identical to or different fromeach other, and each independently represent an arylene group having 6to 20 carbon atoms, an alkylene group having 1 to 10 carbon atoms, abranched alkylene group having 3 to 10 carbon atoms, or an alkylarylenegroup whose alkyl group moiety has 1 to 10 carbon atoms, and may eachcontain, as a functional group, —O—, —COO—, —CO—, —S—, —NH—, or —NR¹¹¹—,R¹¹¹ represents an alkyl group having 1 to 10 carbon atoms or an arylgroup having 6 to 10 carbon atoms, “z” represents 0 or 1, and “b”represents an integer of from 0 to 200.

More specifically, the polyorganosiloxane block (A-1) including therepeating unit represented by the formula (1) preferably includes astructure represented by the following formula (I):

wherein R¹ to R⁴ may be identical to or different from each other, andeach independently represent a hydrogen atom, a halogen atom, an alkylgroup having 1 to 10 carbon atoms, an alkoxy group having 1 to 10 carbonatoms, an aryl group having 6 to 12 carbon atoms, or an alkylaryl groupwhose alkyl group moiety has 1 to 10 carbon atoms, R⁵ and R⁶ may beidentical to or different from each other, and each independentlyrepresent an arylene group having 6 to 20 carbon atoms, an alkylenegroup having 1 to 10 carbon atoms, or an alkylarylene group whose alkylgroup moiety has 1 to 10 carbon atoms, and may each contain, as afunctional group, —O—, —COO—, —CO—, —S—, —NH—, or —NR¹¹¹—, R⁷ and R⁸ maybe identical to or different from each other, and each independentlyrepresent an arylene group having 6 to 20 carbon atoms, an alkylenegroup having 1 to 10 carbon atoms, a branched alkylene group having 3 to10 carbon atoms, or an alkylarylene group whose alkyl group moiety has 1to 10 carbon atoms, and may each contain, as a functional group, —O—,—COO—, —CO—, —S—, —NH—, or —NR″— represents an alkyl group having 1 to10 carbon atoms or an aryl group having 6 to 10 carbon atoms, “z” and“z1” each independently represent 0 or 1, “a” represents an integer offrom 2 to 500, and “b” and “b1” each independently represent an integerof from 0 to 200.

Still more specifically, the polyorganosiloxane block (A-1) includingthe repeating unit represented by the formula (1) preferably has a unitrepresented by any one of the following formulae (I-I) to (I-III):

wherein R¹ to R⁴ may be identical to or different from each other, andeach independently represent a hydrogen atom, a halogen atom, an alkylgroup having 1 to 10 carbon atoms, an alkoxy group having 1 to 10 carbonatoms, an aryl group having 6 to 12 carbon atoms, or an alkylaryl groupwhose alkyl group moiety has 1 to 10 carbon atoms, R⁵ and R⁶ may beidentical to or different from each other, and each independentlyrepresent an arylene group having 6 to 20 carbon atoms, an alkylenegroup having 1 to 10 carbon atoms, or an alkylarylene group whose alkylgroup moiety has 1 to 10 carbon atoms, and may each contain, as afunctional group, —O—, —COO—, —CO—, —S—, —NH—, or —NR¹¹¹—, R⁷ and R⁸ maybe identical to or different from each other, and each independentlyrepresent an arylene group having 6 to 20 carbon atoms, an alkylenegroup having 1 to 10 carbon atoms, a branched alkylene group having 3 to10 carbon atoms, or an alkylarylene group whose alkyl group moiety has 1to 10 carbon atoms, and may each contain, as a functional group, —O—,—COO—, —CO—, —S—, —NH—, or —NR¹¹¹—, R¹¹¹ represents an alkyl grouphaving 1 to 10 carbon atoms or an aryl group having 6 to 10 carbonatoms, “z” and “z1” each independently represent 0 or 1, β represents adivalent group derived from a diisocyanate compound, or a divalent groupderived from a dicarboxylic acid or a dicarboxylic acid halide, “a”represents an integer of from 1 to 500, and represents the average chainlength of the polyorganosiloxane, a-1 represents the number ofrepetitions of a polyorganosiloxane unit, and represents an integer of 2or more, and “b” and “b1” each independently represent an integer offrom 2 to 200.

Preferred examples of R¹ to R⁴, R⁵ and R⁶, R⁷ and R⁸, “z”, “z1”, (3,“a”, “b”, and “b1” in the formula (1), the formula (1A), the formula(3), the formula (I), or the formulae (I-I) to (I-III) are as describedabove. A combination of the preferred examples is also preferred in thepolycarbonate-polyorganosiloxane copolymer.

Among them, such a polycarbonate-polyorganosiloxane copolymer that R¹and R² in the formula (1), or R¹ to R⁴ in the formula (1) and theformula (3) each represent a methyl group is more preferred. Such apolycarbonate-polyorganosiloxane copolymer that in the formula (3), R⁶represents a trimethylene group (—(CH₂)₃—), and/or in the formula (3),R⁸ represents any structure selected from the group consisting of adimethylene group (—(CH₂)₂—), a methyl-substituted dimethylene group(—CH₂CHMe—), a trimethylene group (—(CH₂)₃—), and a tetramethylene group(—(CH₂)₄—) is more preferred.

The average chain length “a” of the polyorganosiloxane block (A-2) inthe polycarbonate-polyorganosiloxane copolymer represents an integer of2 or more and 500 or less, preferably 3 or more and 300 or less, morepreferably 10 or more and 100 or less, still more preferably 15 or moreand 70 or less, still more preferably 20 or more and 65 or less. “a”preferably falls within the ranges because thepolycarbonate-polyorganosiloxane copolymer has a higher total lighttransmittance, and hence serves as a highly transparent copolymer. Theaverage chain length is calculated by nuclear magnetic resonance (NMR)measurement.

The content of the polyorganosiloxane block represented by the formula(1) in the polycarbonate-polyorganosiloxane copolymer is preferably from0.1 mass % to 60 mass %, more preferably from 0.5 mass % to 50 mass %,still more preferably from 1 mass % to 30 mass %, still more preferablyfrom 3 mass % to 20 mass %.

When the content of the polyorganosiloxane block in thepolycarbonate-polyorganosiloxane copolymer falls within the ranges, moreexcellent impact resistance and more excellent transparency can beobtained.

The polycarbonate block (A-2) formed of the repeating unit representedby the formula (2) has a structure derived from the above-mentioned diolmonomer (a1). Specifically, the block preferably has at least oneselected from the group consisting of repeating units represented by thefollowing formulae (a-i) to (a-xiii). The block more preferably has atleast one selected from the group consisting of the repeating unitsrepresented by the following formulae (a-i) to (a-v) in terms oftransparency and an advantage in synthesis, and still more preferablyhas one or more selected from the group consisting of the repeatingunits represented by the following formulae (a-i), (a-ii), and (a-v) interms of higher transparency.

The polycarbonate block (A-2) represented by the formula (2) preferablyincludes a structural unit derived from: an aromatic bisphenol selectedfrom the group consisting of 2,2-bis(4-hydroxyphenyl)propane,2,2-bis(4-hydroxy-3-methylphenyl)propane,1,1-bis(4-hydroxyphenyl)cyclohexane,1,1-bis(4-hydroxyphenyl)-3-methylcyclohexane,1,1-bis(4-hydroxyphenyl)-3,3,5-trimethylcyclohexane, and1,1-bis(4-hydroxyphenyl)cyclododecene; or an aliphatic diol selectedfrom the group consisting of isosorbide, cyclohexane-1,4-dimethanol,tricyclodecanedimethanol,3,9-bis(1,1-dimethyl-2-hydroxyethyl)-2,4,8,10-tetraoxaspiro[5.5]undecane,1,3-propanediol, and 1,4-butanediol.

The polycarbonate block (A-2) formed of the repeating unit representedby the formula (2) more preferably has one or more selected from thegroup consisting of the repeating units represented by the followingformulae (a-i) to (a-v) among them.

“y” representing the number of units of the polycarbonate block (A-2)represented by the formula (2) represents more preferably from 20 to200, still more preferably from 40 to 100. “y” is preferably set to 20or more because an increase in amount of a low-molecular weightcomponent in the resin can be suppressed. “y” is more preferably set to40 or more because the toughness of the resin is improved. “y” ispreferably set to 200 or less because moderate flowability is obtainedat the time of the molding of the resin. “y” is more preferably set to100 or less because a reaction mixture at the time of the production ofthe resin has moderate flowability, and hence productivity is improved.

The polycarbonate-polyorganosiloxane copolymer of the present inventionhas a feature of having high transparency. Specifically, in oneembodiment, a total light transmittance when thepolycarbonate-polyorganosiloxane copolymer of the present invention isturned into a 1-millimeter thick plate can be set to 60% or more. Thetotal light transmittance is a value measured in conformity with ISO13468-1:1996. When the content of the polyorganosiloxane blockrepresented by the formula (1) in the polycarbonate-polyorganosiloxanecopolymer is less than 5 mass %, and the average chain length “a” of thepolyorganosiloxane block (A-2) in the polycarbonate-polyorganosiloxanecopolymer is less than 70, the total light transmittance is morepreferably 70% or more, still more preferably 85% or more, still morepreferably 90% or more. When the content of the polyorganosiloxane blockrepresented by the formula (1) in the polycarbonate-polyorganosiloxanecopolymer is 5 mass % or more, the total light transmittance ispreferably 25% or more.

In one embodiment, the haze value of the 1-millimeter thick plate, whichis obtained by molding the polycarbonate-polyorganosiloxane copolymer ofthe present invention, measured in conformity with ISO 14782:1999 can beset to 40 or less. This is because, as described above, thepolycarbonate-polyorganosiloxane copolymer of the present invention hasa specific structure, and hence has high transparency. The haze value ismore preferably 30 or less, still more preferably 15 or less, still morepreferably 5 or less, particularly preferably 2 or less.

The viscosity-average molecular weight of thepolycarbonate-polyorganosiloxane copolymer of the present invention ispreferably 5,000 or more and 50,000 or less. The viscosity-averagemolecular weight is more preferably 12,000 or more, still morepreferably 14,000 or more, particularly preferably 16,000 or more, andis more preferably 30,000 or less, still more preferably 23,000 or less,particularly preferably 21,000 or less.

The viscosity-average molecular weight (Mv) is a value calculated fromthe following Schnell's equation by measuring the limiting viscosity [η]of a methylene chloride solution (concentration: g/L) at 20° C.

[η]=1.23×10⁻⁵Mv^(0.83)

The polycarbonate-polyorganosiloxane copolymer of the present inventionmay be produced through the polymerization of raw material monomers by amelt polymerization method (ester exchange method). When the copolymeris produced by an interfacial polymerization method, reference may bemade to, for example, a method described in JP 2014-80462 A. Thepolycarbonate-polyorganosiloxane copolymer may be produced by causingthe diol monomer (a1), the polyorganosiloxane (a2), and the carbonicacid ester compound, which are the raw material monomers, to react witheach other in the presence of the basic catalyst, and preferably, achain-end terminator.

(Carbonic Acid Diester)

The carbonic acid diester is at least one kind of compound selected froma diaryl carbonate compound, a dialkyl carbonate compound, and an alkylaryl carbonate compound.

The diaryl carbonate compound is a compound represented by the followingformula (11) or a compound represented by the following formula (12):

wherein

in the formula (11), Ar¹ and Ar² each represent an aryl group, and thegroups may be identical to or different from each other, and in theformula (12), Ara and Ar⁴ each represent an aryl group, and the groupsmay be identical to or different from each other, and D¹ represents aresidue obtained by removing two hydroxyl groups from the aromaticdihydroxy compound or the aliphatic dihydroxy compound.

The dialkyl carbonate compound is a compound represented by thefollowing formula (13) or a compound represented by the followingformula (14):

wherein

in the formula (13), R²¹ and R²² each represent an alkyl group having 1to 20 carbon atoms or a cycloalkyl group having 4 to 20 carbon atoms,and the groups may be identical to or different from each other, and inthe formula (14), R²³ and R²⁴ each represent an alkyl group having 1 to20 carbon atoms or a cycloalkyl group having 4 to 20 carbon atoms, andthe groups may be identical to or different from each other, and D²represents a residue obtained by removing two hydroxyl groups from thearomatic dihydroxy compound or the aliphatic dihydroxy compound.

The alkyl aryl carbonate compound is a compound represented by thefollowing formula (15) or a compound represented by the followingformula (16):

wherein

in the formula (15), Ar⁵ represents an aryl group, and R²⁵ represents analkyl group having 1 to 20 carbon atoms or a cycloalkyl group having 4to 20 carbon atoms, and in the formula (16), Ar⁶ represents an arylgroup, R²⁶ represents an alkyl group having 1 to 20 carbon atoms or acycloalkyl group having 4 to 20 carbon atoms, and D′ represents aresidue obtained by removing two hydroxyl groups from the aromaticdihydroxy compound or the aliphatic dihydroxy compound.

Examples of the diaryl carbonate compound include diphenyl carbonate,ditolyl carbonate, bis(chlorophenyl) carbonate, bis(m-cresyl) carbonate,dinaphthyl carbonate, bis(diphenyl) carbonate, and bisphenol A bisphenylcarbonate.

Examples of the dialkyl carbonate compound include diethyl carbonate,dimethyl carbonate, dibutyl carbonate, dicyclohexyl carbonate, andbisphenol A bismethyl carbonate.

Examples of the alkyl aryl carbonate compound include methyl phenylcarbonate, ethyl phenyl carbonate, butyl phenyl carbonate, cyclohexylphenyl carbonate, and bisphenol A methyl phenyl carbonate.

In the production of the polycarbonate-polyorganosiloxane copolymer ofthe present invention, one kind of the compounds may be, or two or morekinds thereof may each be, appropriately selected and used as thecarbonic acid diester. Among them, diphenyl carbonate is preferablyused.

(Chain-End Terminator)

In the production of the polycarbonate-polyorganosiloxane copolymer ofthe present invention, a chain-end terminator may be used as required.Any known chain-end terminator in the production of a polycarbonateresin may be used as the chain-end terminator. Specific examples thereofmay include the following compounds: phenol, p-cresol,p-tert-butylphenol, p-tert-octylphenol, p-cumylphenol, p-nonylphenol,and p-tert-amylphenol. Those monohydric phenols may be used alone or incombination thereof.

(Branching Agent)

In the production of the polycarbonate-polyorganosiloxane copolymer ofthe present invention, a branching agent may be used. Examples of thebranching agent include: phloroglucin; trimellitic acid;1,1,1-tris(4-hydroxyphenyl)ethane;1-[α-methyl-α-(4′-hydroxyphenyl)ethyl]-4-[α′,α′-bis(4″-hydroxyphenyl)ethyl]benzene;α,α′,α″-tris(4-hydroxyphenyl)-1,3,5-triisopropylbenzene; andisatinbis(o-cresol).

Specifically, the polycarbonate-polyorganosiloxane copolymer of thepresent invention may be produced by the melt polymerization method inaccordance with, for example, the following procedure.

The diol monomer (a1), the polyorganosiloxane (a2), and the carbonicacid ester compound are subjected to an ester exchange reaction. Themolar amount of the carbonic acid ester compound is preferably from 0.9times to 1.2 times, more preferably from 0.98 times to 1.02 times aslarge as that of the diol monomer.

At the time of the ester exchange reaction, the chain-end terminator ispreferably present in an amount within the range of from 0.05 mol % to10 mol % with respect to the diol monomer (a1) and thepolyorganosiloxane (a2) because a hydroxyl group terminal of thepolycarbonate-polyorganosiloxane copolymer to be obtained is sealed, andhence a polycarbonate resin sufficiently excellent in heat resistanceand water resistance is obtained. The total amount of the chain-endterminator may be added to a reaction system in advance, or thefollowing may be adopted: part of the chain-end terminator is added tothe reaction system in advance, and the remainder thereof is addedthereto along with the progress of the reaction.

The ester exchange reaction is preferably performed in the presence ofan antioxidant by simultaneously loading the antioxidant into a reactortogether with the diol monomer (a1), the polyorganosiloxane (a2), andthe carbonic acid ester compound.

When the ester exchange reaction is performed, a reaction temperature isnot particularly limited, and in normal cases, the temperature isselected from the range of from 100° C. to 330° C., preferably from therange of from 180° C. to 300° C., more preferably from the range of from200° C. to 240° C. A method including gradually increasing thetemperature to from 180° C. to 300° C. in accordance with the progressof the reaction is particularly preferred. When the temperature of theester exchange reaction is 100° C. or more, a reaction rate increases.Meanwhile, when the temperature is 330° C. or less, no side reactionoccurs and a problem such as the coloring of thepolycarbonate-polyorganosiloxane copolymer to be produced hardly occurs.

A reaction pressure is set depending on the vapor pressure of a monomerto be used and the reaction temperature. The pressure is notparticularly limited as long as the pressure is set so that the reactionmay be efficiently performed. In normal cases, the following is oftenadopted: at the initial stage of the reaction, the pressure is set to anatmospheric pressure (normal pressure) or pressurized state ranging from1 atm to 50 atm (760 torr to 38,000 torr), and at the later stage of thereaction, the pressure is set to a decompressed state, preferably from1.33 Pa to 1.33×10⁴ Pa (0.01 torr to 100 torr) in the end.

The reaction only needs to be performed until a target molecular weightis obtained, and a reaction time is typically from about 0.2 hour toabout 10 hours.

The ester exchange reaction, which is typically performed in the absenceof an inert solvent, may be performed in the presence of 1 part by massto 150 parts by mass of the inert solvent with respect to 100 parts bymass of the polycarbonate resin to be obtained as required. Examples ofthe inert solvent include: aromatic compounds, such as diphenyl ether,halogenated diphenyl ether, benzophenone, polyphenyl ether,dichlorobenzene, and methylnaphthalene; and cycloalkanes, such astricyclo[5.2.1.0^(2,6)]decane, cyclooctane, and cyclodecane.

The reaction may be performed under an inert gas atmosphere as required,and examples of the inert gas include various gases, such as: gases suchas argon, carbon dioxide, dinitrogen monoxide, and nitrogen;chlorofluorohydrocarbons; alkanes, such as ethane and propane; andalkenes, such as ethylene and propylene.

In the melt polymerization method, the basic catalyst is preferably usedas a catalyst. The basic catalyst may be, for example, at least one kindselected from the group consisting of a metal catalyst, such as analkali metal compound or an alkaline earth metal compound, anitrogen-containing compound, an organic catalyst, such as a quaternaryphosphonium salt containing an aryl group, and a metal compound. Thosecompounds may be used alone or in combination thereof.

As the basic catalyst, there is preferably used, for example, any one ofthe following catalysts: an organic acid salt, an inorganic salt, anoxide, a hydroxide, a hydride, and an alkoxide of an alkali metal or analkaline earth metal; a quaternary ammonium hydroxide; and a quaternaryphosphonium salt containing an aryl group. The basic catalysts may beused alone or in combination thereof.

Examples of the alkali metal compound include sodium hydroxide,potassium hydroxide, cesium hydroxide, lithium hydroxide, sodiumhydrogen carbonate, sodium carbonate, potassium carbonate, cesiumcarbonate, lithium carbonate, sodium acetate, potassium acetate, cesiumacetate, lithium acetate, sodium stearate, potassium stearate, cesiumstearate, lithium stearate, sodium borohydride, sodium benzoate,potassium benzoate, cesium benzoate, lithium benzoate, disodium hydrogenphosphate, dipotassium hydrogen phosphate, dilithium hydrogen phosphate,disodium phenyl phosphate, disodium salt, dipotassium salt, dicesiumsalt, or dilithium salt of bisphenol A, and sodium salt, potassium salt,cesium salt, or lithium salt of phenol.

Example of the alkaline earth metal compound include magnesiumhydroxide, calcium hydroxide, strontium hydroxide, barium hydroxide,magnesium carbonate, calcium carbonate, strontium carbonate, bariumcarbonate, magnesium diacetate, calcium diacetate, strontium diacetate,and barium diacetate.

Examples of the nitrogen-containing compound include: quaternaryammonium hydroxides having an alkyl group, an aryl group, or the like,such as tetramethylammonium hydroxide, tetraethylammonium hydroxide,tetrapropylammonium hydroxide, tetrabutylammonium hydroxide, andtrimethylbenzylammonium hydroxide; tertiary amines, such astriethylamine, dimethylbenzylamine, and triphenylamine; imidazoles, suchas 2-methylimidazole, 2-phenylimidazole, and benzimidazole; and bases orbasic salts, such as ammonia, tetramethylammonium borohydride,tetrabutylammonium borohydride, tetrabutylammonium tetraphenylborate,and tetraphenylammonium tetraphenylborate.

Examples of the metal compound include a zinc-aluminum compound, agermanium compound, an organotin compound, an antimony compound, amanganese compound, a titanium compound, and a zirconium compound.

Specific examples of the quaternary phosphonium salt containing an arylgroup include: tetra(aryl or alkyl)phosphonium hydroxides, such astetraphenylphosphonium hydroxide, tetranaphthylphosphonium hydroxide,tetra(chlorophenyl)phosphonium hydroxide, tetra(biphenyl)phosphoniumhydroxide, tetratolylphosphonium hydroxide, tetramethylphosphoniumhydroxide, tetraethylphosphonium hydroxide, and tetrabutylphosphoniumhydroxide; and tetramethylphosphonium tetraphenylborate,tetraphenylphosphonium bromide, tetraphenylphosphonium phenolate,tetraphenylphosphonium tetraphenylborate, methyltriphenylphosphoniumtetraphenylborate, benzyltriphenylphosphonium tetraphenylborate,biphenyltriphenylphosphonium tetraphenylborate, tetratolylphosphoniumtetraphenylborate, tetraphenylphosphonium phenolate,tetra(p-t-butylphenyl)phosphonium diphenylphosphate,triphenylbutylphosphonium phenolate, and triphenylbutylphosphoniumtetraphenylborate.

The quaternary phosphonium salt containing an aryl group is preferablycombined with a nitrogen-containing organic basic compound, and forexample, a combination of tetramethylammonium hydroxide andtetraphenylphosphonium tetraphenylborate is preferred.

The usage amount of the basic catalyst may be selected from the range ofpreferably from 1×10⁻⁹ mol to 1×10⁻² mol, preferably from 1×10⁻⁸ mol to1×10⁻² mol, more preferably from 1×10⁻⁷ mol to 1×10⁻³ mol with respectto 1 mol of the diol monomer.

A catalyst deactivator may be added at the later stage of the reaction.As the catalyst deactivator to be used, a known catalyst deactivator maybe effectively used, and among them, ammonium salts or phosphonium saltsof sulfonic acid are preferred. Further, salts of dodecylbenzenesulfonicacid, such as tetrabutylphosphonium dodecylbenzenesulfonate, or salts ofp-toluenesulfonic acid, such as tetrabutylammonium p-toluenesulfonate,are preferred.

As esters of sulfonic acid, methyl benzenesulfonate, ethylbenzenesulfonate, butyl benzenesulfonate, octyl benzenesulfonate, phenylbenzenesulfonate, methyl p-toluenesulfonate, ethyl p-toluenesulfonate,butyl p-toluenesulfonate, octyl p-toluenesulfonate, phenylp-toluenesulfonate, and the like are also preferably used. Among them,tetrabutylphosphonium dodecylbenzenesulfonate or butylp-toluenesulfonate is most preferably used.

With regard to the usage amount of the catalyst deactivator, when atleast one kind of polymerization catalyst selected from alkali metalcompounds and alkaline earth metal compounds is used, the catalystdeactivator may be used preferably at a ratio of from 0.5 mol to 50 mol,more preferably at a ratio of from 0.5 mol to 10 mol, still morepreferably at a ratio of from 0.8 mol to 5 mol per 1 mol of thecatalyst.

The antioxidant is preferably mixed after the catalyst deactivator hasbeen added to terminate the polymerization reaction.

The reaction in the melt polymerization method may be performed by anyone of a continuous system and a batch system. A reactor to be used inmelt polymerization may be any one of: a vertical reactor equipped with,for example, an anchor-type stirring blade, a max blend stirring blade,or a helical ribbon-type stirring blade; and a horizontal reactorequipped with, for example, a paddle blade, a lattice blade, or aspectacle blade. Further, the reactor may be of an extruder typeequipped with a screw. In the case of the continuous system, anappropriate combination of such reactors is preferably used.

At the time of the production of the polycarbonate-polyorganosiloxanecopolymer of the present invention, as described above, the mixture,which is formed of the diol monomer (a1), the polyorganosiloxane (a2),and the carbonic acid ester compound, and is obtained by bringing thediol monomer (a1), the polyorganosiloxane (a2), the carbonic acid estercompound, and the basic catalyst into contact with each other at from100° C. to 250° C. for from 0.5 hour to 5 hours, needs to have a hazevalue of 30 or less measured under the conditions of 23° C. and anoptical path length of 10 mm in conformity with ISO 14782:1999.

Although the refractive index of the polycarbonate-polyorganosiloxanecopolymer of the present invention is not particularly limited, forexample, the refractive index thereof for light having a wavelength of589.3 nm is preferably 1.430 or more and 1.590 or less, more preferably1.450 or more and 1.570 or less, still more preferably 1.470 or more and1.550 or less.

A difference (nF-nC) between the refractive index (nF) of thepolycarbonate resin for light having a wavelength of 486.1 nm and therefractive index (nC) thereof for light having a wavelength of 656.3 nmis preferably 0.015 or less, more preferably 0.013 or less, still morepreferably 0.011 or less.

<Polycarbonate-Based Resin Composition>

The polycarbonate-based resin composition of the present inventionincludes the above-mentioned polycarbonate-polyorganosiloxane copolymer(polycarbonate-polyorganosiloxane copolymer (A)).

A known additive may be used in the polycarbonate-based resincomposition of the present invention as long as the characteristics ofthe polycarbonate-polyorganosiloxane copolymer (A) are not impaired.

(Additive)

A known additive may be blended into the polycarbonate-based resincomposition of the present invention in accordance with its applicationsor as required. Examples of the additive include various fillers, anantioxidant, a heat stabilizer, a plasticizer, a light stabilizer, apolymerization metal deactivator, a flame retardant, a lubricant, anantistatic agent, a surfactant, an antimicrobial agent, a UV absorber,and a release agent.

The antioxidant can suppress the decomposition of a resin at the time ofthe production or molding of a thermoplastic resin composition.

[Filler]

The filler that may be blended into the polycarbonate-based resincomposition of the present invention is, for example, an inorganicfiller, such as a spherical filler, a plate-like filler, or a fibrousfiller.

Examples of the spherical filler include calcium carbonate, kaolin(aluminum silicate), silica, pearlite, shirasu balloons, sericite,diatomaceous earth, calcium sulfite, calcined alumina, calcium silicate,crystalline zeolite, and amorphous zeolite.

Examples of the plate-like filler include talc, mica, and wollastonite.

Examples of the fibrous filler include: needle-like fillers, such as aglass fiber, a carbon fiber, and wollastonite; and fibrous fillers, suchas magnesium oxysulfate, a potassium titanate fiber, and fibrous calciumcarbonate. The inorganic filler is preferably a glass fiber or a carbonfiber.

Fibers each using any one of, for example, an alkali glass, a low-alkaliglass, and a non-alkali glass as a raw material may each be suitablyused as the glass fiber.

The forms of those glass fibers are not particularly limited, and fibersof any forms, such as a roving, a milled fiber, and a chopped strand,may be used.

A commercial product of the glass fiber is, for example, CSH-3PA(manufactured by Nitto Boseki Co., Ltd.), T-511 (manufactured by NipponElectric Glass Co., Ltd.), or MA-409C (manufactured by Asahi Fiber GlassCo., Ltd.).

The polycarbonate-based resin composition of the present inventionpreferably includes a glass filler from the viewpoint of reinforcing theresin composition.

Although the refractive index of the glass filler is not particularlylimited, for example, the refractive index thereof at a wavelength of589.3 nm is preferably from 1.485 to 1.520. When the refractive index ofthe glass filler falls within the range, the transparency of a moldedbody obtained by using the polycarbonate-based resin composition of thepresent invention can be improved.

Further, from the viewpoint of improving the transparency of the moldedbody formed of the polycarbonate-based resin composition, the refractiveindex of the glass filler at a wavelength of 589.3 nm is more preferably1.490 or more, still more preferably 1.500 or more, and is morepreferably 1.515 or less, still more preferably 1.514 or less.

[Composition Ratio]

The polycarbonate-based resin composition of the present invention mayinclude preferably 1 part by mass to 150 parts by mass, more preferably11 parts by mass to 100 parts by mass, still more preferably 15 parts bymass to 60 parts by mass, still more preferably 15 parts by mass to 40parts by mass of the inorganic filler with respect to 100 parts by massof the polycarbonate-polyorganosiloxane copolymer (A). When the contentis set within the ranges, various mechanical property-improving effectsresulting from the inorganic filler, for example, an improvement instrength, such as an elastic modulus, can be achieved without theimpairment of the characteristics of thepolycarbonate-polyorganosiloxane copolymer (A).

A method of producing the polycarbonate-based resin composition of thepresent invention is not particularly limited as long as the methodincludes a step of mixing the polycarbonate-polyorganosiloxane copolymerand an optional additive. The composition may be produced by, forexample, mixing the polycarbonate-polyorganosiloxane copolymer and theoptional additive with a mixer or the like, and melting and kneading themixture. The melting and kneading may be performed by a method that hasbeen typically employed, for example, a method including using a ribbonblender, a Henschel mixer, a Banbury mixer, a drum tumbler, asingle-screw extruder, a twin-screw extruder, a co-kneader, amulti-screw extruder, or the like. A heating temperature at the time ofthe melting and kneading is appropriately selected from the range oftypically from about 150° C. to about 300° C., preferably from about220° C. to about 300° C.

[Molded Article]

A molded article of the present invention includes thepolycarbonate-based resin composition of the present invention. Themolded article may be produced through use of a melt-kneaded product ofthe polycarbonate-based resin composition or a pellet thereof obtainedthrough melting and kneading as a raw material by any one of, forexample, an injection molding method, an injection compression moldingmethod, an extrusion molding method, a blow molding method, a pressmolding method, a vacuum molding method, and an expansion moldingmethod. In particular, the molded article is preferably produced throughuse of the resultant pellet by the injection molding method or theinjection compression molding method.

The thickness of the molded article may be arbitrarily set in accordancewith its applications. In particular, when the transparency of themolded article is required, the thickness is preferably from 0.2 mm to4.0 mm, more preferably from 0.3 mm to 3.0 mm, still more preferablyfrom 0.3 mm to 2.0 mm. When the thickness of the molded article is 0.2mm or more, its warping does not occur and good mechanical strength isobtained. In addition, when the thickness of the molded article is 4.0mm or less, high transparency is obtained.

A coating film formed of a hard coating film, an antifogging film, anantistatic film, or an antireflection film may be formed on the moldedarticle as required, and a composite coating film formed of two or morekinds thereof may be formed.

Among them, a coating film formed of a hard coating film is particularlypreferably formed because the film has good weatherability and canprevent the wear of the surface of the molded article with time. Amaterial for the hard coating film is not particularly limited, and aknown material, such as an acrylate-based hard coating agent, asilicone-based hard coating agent, or an inorganic hard coating agent,may be used.

In the case of a molded article including a glass filler, when at leastpart of the glass filler is present on the outermost surface of themolded article, the surface roughness of the molded article increasesand the degree of irregular reflection at the surface of the moldedarticle increases, and as a result, the transparency of the moldedarticle deteriorates in some cases. In view of the foregoing, forexample, a method including forming a layer containing a high proportionof the resin (skin layer) on the outermost surface of the molded articleto reduce the surface roughness of the molded article is available as amethod of reducing the surface roughness of the molded article. In thecase of injection molding, a method of forming the skin layer mayinclude setting the temperature of a mold to a temperature higher than ageneral condition to allow the resin in contact with the mold to easilyflow, thereby reducing the surface roughness of the outermost surface ofthe molded article. In addition, in the case of compression molding,when a pressure at the time of the molding is set to a pressure higherthan a general condition, the surface roughness of the outermost surfaceof the molded article can be reduced. When the surface roughness of themolded article is reduced by employing any such method, the irregularreflection at the surface of the molded article is suppressed and a hazereduces, and as a result, the transparency of the molded article can beimproved.

When the molded article thus obtained is molded into a flat plate, theflat plate preferably has a total light transmittance for visible lightof 60% or more in the case where the content of the polyorganosiloxaneblock represented by the formula (1) in thepolycarbonate-polyorganosiloxane copolymer is less than 5 mass %, andthe average chain length “a” of the polyorganosiloxane block (A-2) inthe polycarbonate-polyorganosiloxane copolymer is less than 70. Thetotal light transmittance is more preferably 70% or more, still morepreferably 80% or more, still more preferably 85% or more, still morepreferably 90% or more. When the content of the polyorganosiloxane blockrepresented by the formula (1) in the polycarbonate-polyorganosiloxanecopolymer is 5 mass % or more, the total light transmittance for visiblelight is preferably 25% or more. When the content of thepolyorganosiloxane block represented by the formula (1) in thepolycarbonate-polyorganosiloxane copolymer is less than 5 mass %, andthe average chain length “a” of the polyorganosiloxane block (A-2) inthe polycarbonate-polyorganosiloxane copolymer is less than 70, the hazeof the molded article when molded into the flat plate is preferably 40or less, more preferably 30 or less, still more preferably 15 or less,still more preferably 5 or less, particularly preferably 2 or less.

The molded article having the above-mentioned optical properties may beused in an application where high transparency is required because themolded article is excellent in transparency. The total lighttransmittance for visible light may be measured in conformity with ISO13468-1:1996, and the haze may be measured in conformity with ISO14782:1999.

The molded article including the polycarbonate resin according to thepresent invention can be suitably used in members that are each requiredto have transparency and rigidity, and further, scratch resistance andweatherability, such as: 1) automobile parts, such as a sunroof, a doorvisor, a rear window, and a side window; 2) building parts, such as abuilding glass, a soundproof wall, a car port, a sunroom, and gratings;3) windows for railway vehicles and ships; 4) parts for electricalinstruments, such as various parts for a television, a radio-cassetterecorder, a video camera, a video tape recorder, an audio player, a DVDplayer, a telephone, a display, a computer, a register, a copyingmachine, a printer, a facsimile, and the like, and respective parts forouter plates and housings thereof; 5) parts for precision instruments,such as casings and covers for precision machines, such as a cellularphone, a PDA, a camera, a slide projector, a watch, an electroniccalculator, a measuring instrument, and a display instrument; 6)agricultural parts, such as a vinyl house and a greenhouse; and 7)furniture parts, such as a lighting cover, blinds, and interior tools.

EXAMPLES

The present invention is described in more detail below by way ofExamples, but the present invention is not limited to these Examples.

Characteristic values in the respective examples were determined inaccordance with the following procedures.

<Method of Determining Polydimethylsiloxane Content>

(Example) Method of determining Amount of Polydimethylsiloxane inPolycarbonate-polyorganosiloxane Copolymer obtained in Example 3

NMR apparatus: ECA-500 manufactured by JEOL RESONANCE Inc.

Probe: TH 5 corresponding to a 5 φ NMR sample tube

Observation range: From −5 ppm to 15 ppm

Observation center: 5 ppm

Pulse repetition time: 9 seconds

Pulse width: 45°

Number of scans: 256 times

NMR sample tube: 5 φ

Sample amount: From 30 mg to 40 mg

Solvent: Deuterated chloroform

Measurement temperature: Room temperature

A: The integrated value of the meta position of a phenyl moiety observedat a δ of from about 7.3 to about 7.5

B: The integrated value of a methyl group of a dimethylsiloxane moietyobserved at a δ of from about −0.02 to about 0.3

C: The integrated value of a methine group of an isosorbide (ISB) moietyobserved at a δ of from about 4.8 to about 5.3

D: The integrated value of a methylene group of a PEG moiety observed ata δ of from about 3.3 to about 3.8

E: The integrated value of a methine group and a methylene group of aCHDM moiety observed at a δ of from about 0.8 to about 2.0

F: The integrated value of a methylene group of a dimethylsiloxaneterminal moiety observed at a δ of from about 0.4 to about 0.6

a=A/2

b=B/6

c=C/3

d=D/4

e=(E−F)/10

T=a+b+c+d+e

f=a/T×100

g=b/T×100

h=c/T×100

i=d/T×100

j=e/T×100

TW=f×93+g×74.1+h×172+i×44+j×170

PDMS (wt %)=g×74.1/TW×100

<Viscosity-Average Molecular Weight of Polycarbonate-PolyorganosiloxaneCopolymer>

A viscosity-average molecular weight (Mv) was calculated from thefollowing equation (Schnell's equation) by using a limiting viscosity[η] determined through the measurement of the viscosity of a methylenechloride solution (concentration: g/L) at 20° C. with an Ubbelohde-typeviscometer.

[η]=1.23×10⁻⁵ Mv^(0.83)

[Evaluation Test] <Total Light Transmittance Tt (%) and Haze Value ofResin Molded Article>

An evaluation pellet obtained in each of Examples and ComparativeExamples was molded with an injection molding machine (manufactured byNiigata Machine Techno Co., Ltd., “MD50XB”, screw diameter: 30 mmφ) at acylinder temperature of 240° C. and a mold temperature of 80° C. into athree-stage plate for a transparency evaluation (90 mm×50 mm,3-millimeter thick portion: 45 mm×50 mm, 2-millimeter thick portion:22.5 mm×50 mm, 1-millimeter thick portion: 22.5 mm×50 mm). The totallight transmittance of the 1-millimeter thick portion of the three-stageplate was measured in conformity with ISO 13468-1:1996. The haze valueof the 1-millimeter thick portion of the same sample was measured inconformity with ISO 14782:1999. Both the values were measured by usingNDH 5000 manufactured by Nippon Denshoku Industries Co., Ltd. as ameasuring apparatus.

A smaller haze value means that the transparency of the sample ishigher.

Haze=Td/Tt×100

wherein Td represents the diffuse transmittance of the sample, and Ttrepresents the total light transmittance thereof.

<Total Light Transmittance (%) and Haze Value of Raw Material Mixture>

The total light transmittance and haze value of a raw material mixturewere determined by using the following measuring apparatus, glass cell,and measurement method.

Measuring apparatus: NDH 5000 manufactured by Nippon Denshoku IndustriesCo., Ltd.

Glass cell: Optical path length: 10 mm

Dimensions: External dimensions measuring 14 mm (length)×40 mm(width)×55 mm (height)

Glass thickness of each surface: 2 mm

Prior to the measurement of the haze of the raw material mixture,zero-point adjustment was performed by filling the glass cell with purewater. Specifically, the adjustment was performed so that the followingstates were established: the measured value of a total lighttransmittance in a state in which the cell was filled with the purewater became 100%; and the measured value of a haze value in the statebecame 0.00. Next, the pure water was removed from the glass cell, andthe cell was filled with a liquid mixture obtained by a method to bedescribed later and subjected to measurement, followed by thedetermination of the haze value of the mixture at 23° C. in conformitywith ISO 14782:1999.

Haze=Td/Tt×100

wherein Td represents the diffuse transmittance of the mixture, and Ttrepresents the total light transmittance thereof.

Production Example 1: Production of PDMS-1

Under a nitrogen atmosphere, to a polyorganosiloxane (100 g) having asiloxane average chain length of 24, which was represented by thefollowing formula:

a polyethylene glycol having an average oxyethylene chain length of 15,which was represented by the following formula:

H₂C═CH—CH₂—O—(CH₂CH₂O)₁₅—H

was added in a molar amount (82.3 g) twice as large as that of thepolyorganosiloxane. 455 Grams (2.5 parts with respect to the total massof the polyorganosiloxane and the polyethylene glycol) of isopropylalcohol was added to the materials, and then the mixture wassufficiently stirred while its temperature was controlled to 80° C.Next, a solution of a vinylsiloxane complex of platinum in toluene wasadded to the mixture in such an amount that the mass of a platinum atombecame 5 ppm by mass with respect to the siloxane, followed by stirringfor 10 hours. Isopropyl alcohol and the platinum catalyst were removedfrom the resultant mixture. Thus, a polyether-modifiedpolyorganosiloxane PDMS-1 was obtained.

Production Example 2: Production of PDMS-2

Production was performed in the same manner as in Production Example 1except that an α,ω-dihydrogen organopolysiloxane having an averagesiloxane chain length of 61 was used.

Production Example 3: Production of PDMS-3

Production was performed in the same manner as in Production Example 1except that an α,ω-dihydrogen organopolysiloxane having an averagesiloxane chain length of 88 was used.

Production Example 4: Production of PDMS-4

Production was performed in the same manner as in Production Example 1except that the average oxyethylene chain length of the polyethyleneglycol to be used was set to 12.

Production Example 5: Production of PDMS-5

Under a nitrogen atmosphere, to a polyorganosiloxane having an averagesiloxane chain length of 39, which was represented by the followingformula:

2-allylphenol was added in a molar amount twice as large as that of thepolyorganosiloxane. The mixture was sufficiently stirred while itstemperature was controlled to 100° C. Next, a solution of avinylsiloxane complex of platinum in toluene was added to the mixture insuch an amount that the mass of a platinum atom became 5 ppm by masswith respect to the siloxane, followed by stirring for 10 hours.Isopropyl alcohol and the platinum catalyst were removed from theresultant mixture. Thus, an allylphenol-modified polyorganosiloxanePDMS-5 was obtained.

Production Example 6: Production of PDMS-6

Production was performed in the same manner as in Production Example 5except that eugenol was used instead of 2-allylphenol.

Production Example 7: Production of PDMS-7

Production was performed in the same manner as in Production Example 1except that ethylene glycol monoallyl ether (CH₂═CHCH₂—O—CH₂CH₂—OH) wasused instead of the polyethylene glycol.

Production Example 8: Production of PDMS-8

Production was performed in the same manner as in Production Example 1except that: the siloxane average chain length of the polyorganosiloxaneto be used was set to 45; the average oxyethylene chain length of thepolyethylene glycol to be used was set to 8; toluene was used as asolvent; and the reaction temperature was set to 110° C.

Production Example 9: Production of PDMS-9

Production was performed in the same manner as in Production Example 8except that: the average oxyethylene chain length of the polyethyleneglycol to be used was set to 38; toluene was used as a solvent; and thereaction temperature was set to 110° C.

Production Example 10: Production of PDMS-10

Production was performed in the same manner as in Production Example 1except that: the siloxane average chain length of the polyorganosiloxaneto be used was set to 5; toluene was used as a solvent; and the reactiontemperature was set to 110° C.

Production Example 11: Production of PDMS-11

Under a nitrogen atmosphere, 350 mL of methylene chloride was loadedinto a flask, and 21.5 g of 2,6-di-t-butylpyridine and 21 g oftrifluoromethanesulfonic anhydride were loaded into the flask, followedby the cooling of the mixture to 15° C. or less. 4.3 Grams of allylalcohol was dropped into the mixture to form a reaction initiator. Afterthe initiator had been stirred for about 15 minutes, 1 L of dehydratedtetrahydrofuran was loaded into the initiator, and the mixture wasstirred at from 20° C. to 23° C. for 5 minutes. After that, 30 mL ofion-exchanged water was loaded into the mixture to terminate thereaction. The resultant was extracted with heptane and washed with 10%hydrochloric acid, followed by the separation of an aqueous phase. Afterthat, the residue was subsequently washed with ion-exchanged watertwice, and an aqueous phase was separated. After that, the solvent wasevaporated under a decompressed condition. Thus, 120 g of a one-terminalallyl-modified polytetramethylene glycol (chain length of itstetramethylene glycol moiety=20) represented by the following formulawas obtained.

H₂C═CH—CH₂—(OCH₂CH₂CH₂CH₂)₂₀—OH

Production was performed in the same manner as in Production Example 8except that: the one-terminal allyl-modified polytetramethylene glycolobtained by the above-mentioned reaction was used instead of thepolyethylene glycol; the solvent was changed to a mixed liquidcontaining toluene and isopropanol at 1:1 (mass ratio), and the usageamount of the solvent was set to a volume amount three times as large asthe total volume of the polyorganosiloxane and the one-terminalallyl-modified polytetramethylene glycol; and the reaction temperaturewas controlled to from 80° C. to 90° C.

Production Example 12: Production of PDMS-12

A polydimethylsiloxane having —C₃H₆OC₂H₄OH groups at both of itsterminals (average chain number of a SiMe₂O unit: 40) and trimethylenecarbonate whose molar amount was 25 times as large as that of thehydroxyl groups of the above-mentioned polyorganosiloxane were loadedinto a flask under a nitrogen atmosphere, and dehydrated dichloromethanewas loaded into the flask so that the concentration of the raw materialsbecame 10 wt %. 3 Equivalents of 1,8-diazabicycloundecene with respectto the terminal OH groups of the polydimethylsiloxane was loaded as acatalyst into the resultant transparent reaction solution, and themixture was subjected as it was to a reaction under room temperature for48 hours. After that, benzoic acid was added to terminate the reaction,and the resultant reaction mixture was reprecipitated in a mixed solventformed of a mixed liquid containing methanol, 2-propanol, and hexane (ata volume ratio of 10:1:10). The resultant precipitate was vacuum-driedto provide a PDMS-12 (chain number of polytrimethylene carbonate at eachterminal: 18).

Production Example 13: Production of PDMS-13

Under a nitrogen atmosphere, 450 mL of methylene chloride was loadedinto a flask, and 45.0 g of 3-iodo-1-propanol was added to the flask,followed by the cooling of the mixture with an ice bath. 40.1 Grams oftert-butyldimethylchlorosilane was added to the mixture, and the wholewas stirred under room temperature for 20 hours. The resultant mixturewas quenched with a 5% aqueous solution of sodium hydrogen carbonate,and the product was extracted with an ethyl acetate/ion-exchanged watersystem. The resultant product was purified with a silica gel column toprovide the TBS-protected form of 3-iodo-1-propanol (yield: 67.7 g).

Under a nitrogen atmosphere, 2.9 g of the above-mentioned TB S-protectedform of 3-iodo-1-propanol and 270 mL of tetrahydrofuran were mixed in aflask, and the mixture was cooled to −65° C. or less. 12.5 Millilitersof 1.6 mol/L tert-butyllithium (pentane solution) was dropped into themixture, and the whole was stirred as it was for 15 minutes. 2.5Milliliters of diphenylethylene was dropped into the resultant, and themixture was stirred as it was for 30 minutes. After that, 55 mL of a0.52 mol/L solution of lithium chloride in THF was loaded into themixture, and the whole was stirred for 10 minutes. Next, 10.1 mL ofmethyl methacrylate was loaded into the resultant, and the mixture wasstirred for 10 minutes. Next, 3.36 mL of allyl bromide was loaded toquench the reaction, and then the contents in the flask were mixed atroom temperature for 12 hours. The resultant reaction mixture wasconcentrated under reduced pressure, and then the concentrate wasreprecipitated in a THF/heptane system. After that, the precipitate waspurified with a silica gel column so that the solvent was removed. Thus,the TB S-protected form of a one-terminal allyl-modified polymethylmethacrylate (PMMA) was obtained. The product was dissolved in THF, andwas deprotected with a 2 mol/L aqueous solution of hydrochloric acid.The resultant reaction mixture was loaded into heptane so that a targetproduct (deprotected form) was separated. The deprotected form waspurified with a silica gel column so that the solvent was removed. Thus,the one-terminal allyl-modified PMMA (chain number of its PMMAmoiety=20) represented by the following formula was obtained.

Production was performed in the same manner as in Production Example 8except that the above-mentioned one-terminal allyl-modified PMMA wasused instead of the polyethylene glycol.

Production Example 14: Production of PDMS-14

Production was performed in the same manner as in Production Example 1except that a polypropylene glycol having an average oxypropylene chainlength of 15, which was represented by the following formula:

was used instead of the polyethylene glycol.

The PDMS-1 to the PDMS-14 obtained in Production Examples 1 to 14 areshown in Table 1.

TABLE 1 Production Example 1

Production Example 2

Production Example 3

Production Example 4

Production Example 5

Production Example 6

Production Example 7

Production Example 8

Production Example 9

Production Example 10

Production Example 11

Production Example 12

Production Example 13

Production Example 14

[Others]

BisP-A: bisphenol A [manufactured by Idemitsu Kosan Co., Ltd.]

1,4-CHDM: 1,4-cyclohexanedimethanol [manufactured by Tokyo ChemicalIndustry Co., Ltd.]

TCDDM: tricyclodecanedimethanol [manufactured by OXEA GmbH]

1,3-PG: 1,3-propanediol [manufactured by Tokyo Chemical Industry Co.,Ltd.]

PEG 400: polyethylene glycol 400 [average molecular weight: 380 g/mol to420 g/mol, manufactured by Tokyo Chemical Industry Co., Ltd.]

DPC: diphenyl carbonate [manufactured by Mitsui Fine Chemicals, Inc.]

0.01 N sodium hydroxide aqueous solution [manufactured by Fujifilm WakoPure Chemical Corporation]

Example 1

<Evaluation of Transparency of Raw Material Mixture after its HeatingTreatment>

BisP-A (2,489.9 g) and DPC (2,500 g) (molar ratio between the respectiveraw materials: BisP-A/DPC=100/107), and 28.2 g of the polyether-modifiedpolyorganosiloxane PDMS-1 were loaded into a 10-liter stainlesssteel-made reactor including a double helical blade as a stirringapparatus. Those raw material monomers were completely melted at 150°C., and then the stirring of the molten product was started at 70 rpm,followed by the purging of air in the reactor with nitrogen. Next, 1.64mL (amount 1.5×10⁻⁶ times as large as the number of moles of the entirediol monomer) of 0.01 N sodium hydroxide was loaded as a catalyst intothe reactor. While the pressure of nitrogen was held at 101 kPa equal toatmospheric pressure, the temperature of the mixture was increased to200° C., and the temperature was held for 60 minutes. Subsequently, thecontents were extracted from a valve in the bottom portion of thereactor to provide a liquid and transparent raw material mixture. Theliquid raw material mixture after its heating treatment had a totallight transmittance of 98.4% and a haze value of 0.5, and hence showedhigh transparency.

<Production of Polycarbonate-polyorganosiloxane (PC-POS) Copolymer>

A polycarbonate-polyorganosiloxane copolymer was produced by using thefollowing raw materials under the following conditions. The same rawmaterials as those subjected to the transparency evaluation are used asthe raw materials, and their polymerization conditions are as describedbelow.

BisP-A (2,489.9 g) serving as a diol monomer and DPC (2,500 g) (molarratio between the respective raw materials: BisP-A/DPC=100/107), and28.2 g of the polyether-modified polyorganosiloxane PDMS-1 were loadedinto a 10-liter stainless steel-made reactor including a stirringapparatus, a trap configured to trap distilled phenol, and adecompression apparatus, and these raw material monomers were completelymelted at 150° C., followed by the purging of air in the reactor withnitrogen. 1.64 Milliliters (amount 1.5×10⁻⁶ times as large as the numberof moles of the entire diol monomer) of 0.01 N sodium hydroxide wasloaded as a catalyst into the reactor to initiate polymerization. Atemperature in the reactor was increased to 180° C., and the reactor wasdecompressed to a decompression degree of 200 mmHg (26.6 kPa), overabout 60 minutes, and the reaction conditions were held until the amountof phenol to be distilled out became 0.2 L. After that, the temperaturein the reactor was increased to 200° C., and the reactor wasdecompressed to a decompression degree of 10 mmHg (1.3 kPa), over about60 minutes, and the conditions were held until 1.0 L of phenol wasdistilled out.

Next, the temperature in the reactor was increased to 240° C. over about120 minutes, and the condition was held until 1.5 L of phenol wasdistilled out. Subsequently, the temperature and the decompressiondegree in the reactor were adjusted to 280° C. and 1 mmHg (0.1 kPa) orless, respectively over about 120 minutes. Two liters or more of phenolwas distilled out, and the reaction was continued until a predeterminedstirring torque was obtained. After that, the pressure in the reactorwas returned to atmospheric pressure with nitrogen, and 0.037 g (amount10 times as large as the number of moles of NaOH) of butylp-toluenesulfonate was loaded as a deactivator into the reactor. Each ofIrganox 1010 and Irgafos 168 was loaded into the reactor so that itscontent in a polymer to be obtained became 1,500 ppm, followed bysufficient stirring. After that, a resin strand was extracted from thebottom portion of the reactor with the pressure of nitrogen, and thestrand was cut with a pelletizer to provide a pellet-shapedpolycarbonate-polyorganosiloxane copolymer having high transparency. Theresults of the evaluations of the resultantpolycarbonate-polyorganosiloxane copolymer are shown in Table 2.

Example 2

The transparency of a raw material mixture after its heating treatmentwas evaluated in the same manner as in Example 1 except that BisP-A(1,293.3 g) and 1,4-CHDM (817.0 g) serving as diol monomers, and DPC(2,500 g) (molar ratio among the respective raw materials:BisP-A/1,4-CHDM/DPC=50/50/103), and 24.4 g of the polyether-modifiedpolyorganosiloxane PDMS-1 were used. The liquid raw material mixtureafter the heating treatment had high transparency, and had a total lighttransmittance of 98.5% and a haze value of 0.5.

Polymerization was performed under the same conditions as those ofExample 1 except that BisP-A (1,293.3 g) and 1,4-CHDM (817.0 g) servingas diol monomers, and DPC (2,500 g) (molar ratio among the respectiveraw materials: BisP-A/1,4-CHDM/DPC=50/50/103), and 24.4 g of thepolyether-modified polyorganosiloxane PDMS-1 were used. Thus, apellet-shaped polycarbonate-polyorganosiloxane copolymer having hightransparency was obtained. The results of the evaluations of theresultant polycarbonate-polyorganosiloxane copolymer are shown in Table2.

Example 3

<Evaluation of Transparency of Raw Material Mixture after its HeatingTreatment>

The heating treatment of raw materials was performed in the same manneras in Example 1 except that isosorbide (ISB) (1,193.8 g), 1,4-CHDM(504.9 g), and DPC (2,500 g) (molar ratio among the respective rawmaterials: ISB/1,4-CHDM/DPC=70:30:100), and 20.2 g of thepolyether-modified polyorganosiloxane PDMS-1 were used. The liquid rawmaterial mixture after the heating treatment had high transparency, andhad a total light transmittance of 99.5% and a haze value of 0.4.

<Production of PC-POS Copolymer>

ISB (1,193.8 g) and 1,4-CHDM (504.9 g) serving as diol monomers, and DPC(2,500 g) (molar ratio among the respective raw materials:ISB/1,4-CHDM/DPC=70:30:100), and 20.2 g of the polyether-modifiedpolyorganosiloxane PDMS-1 were loaded into a 10-liter stainlesssteel-made reactor including a stirring apparatus, a trap configured totrap distilled phenol, and a decompression apparatus, and these rawmaterial monomers were completely melted at 100° C., followed by thepurging of air in the reactor with nitrogen. 1.64 Milliliters (amount1.5×10⁻⁶ times as large as the number of moles of all the diol monomers)of 0.01 N sodium hydroxide was loaded as a catalyst into the reactor toinitiate polymerization. A temperature in the reactor was increased to180° C., and the reactor was decompressed to a decompression degree of200 mmHg (26.6 kPa), over from about 50 minutes to about 100 minutes,and the conditions were held until the amount of phenol to be distilledout became 0.2 L. After that, the temperature in the reactor wasincreased to 200° C., and the reactor was decompressed to adecompression degree of 10 mmHg (1.3 kPa), over about 150 minutes, andthe conditions were held until 1.8 L of phenol was distilled out.

Next, the temperature and the decompression degree in the reactor wereadjusted to 220° C. and 1 mmHg (0.1 kPa) or less, respectively overabout 60 minutes. Two liters or more of phenol was distilled out, andthe reaction was continued until a predetermined stirring torque wasobtained. After that, the pressure in the reactor was returned toatmospheric pressure with nitrogen, and 0.037 g (amount 10 times aslarge as the number of moles of NaOH) of butyl p-toluenesulfonate wasloaded as a deactivator into the reactor. Each of Irganox 1010 andIrgafos 168 was loaded into the reactor so that its content in a polymerto be obtained became 1,500 ppm, followed by sufficient stirring. Afterthat, a resin strand was extracted from the bottom portion of thereactor with the pressure of nitrogen, and the strand was cut with apelletizer to provide a pellet-shaped polycarbonate-polyorganosiloxanecopolymer having high transparency. The results of the evaluations ofthe resultant polycarbonate-polyorganosiloxane copolymer are shown inTable 2.

Example 4

The transparency of a raw material mixture after its heating treatmentwas evaluated in the same manner as in Example 3 except that 20.2 g ofthe PDMS-2 was used as a polyorganosiloxane. The liquid raw materialmixture after the heating treatment had high transparency, and had atotal light transmittance of 98.4% and a haze value of 0.8.

Polymerization was performed under the same conditions as those ofExample 3 except that 20.2 g of the PDMS-2 was used as apolyorganosiloxane. Thus, a pellet-shapedpolycarbonate-polyorganosiloxane copolymer having high transparency wasobtained. The results of the evaluations of the resultantpolycarbonate-polyorganosiloxane copolymer are shown in Table 2.

Example 5

The transparency of a raw material mixture after its heating treatmentwas evaluated in the same manner as in Example 3 except that 20.2 g ofthe PDMS-3 was used as a polyorganosiloxane. The liquid raw materialmixture after the heating treatment had high transparency, and had atotal light transmittance of 98.1% and a haze value of 1.3.

Polymerization was performed under the same conditions as those ofExample 3 except that 20.2 g of the PDMS-3 was used as apolyorganosiloxane. Thus, a pellet-shapedpolycarbonate-polyorganosiloxane copolymer having high transparency wasobtained. The results of the evaluations of the resultantpolycarbonate-polyorganosiloxane copolymer are shown in Table 2.

Example 6

The transparency of a raw material mixture after its heating treatmentwas evaluated in the same manner as in Example 3 except that 20.2 g ofthe PDMS-4 was used as a polyorganosiloxane. The liquid raw materialmixture after the heating treatment had high transparency, and had atotal light transmittance of 97.9% and a haze value of 0.7.

Polymerization was performed under the same conditions as those ofExample 3 except that 20.2 g of the PDMS-4 was used as apolyorganosiloxane. Thus, a pellet-shapedpolycarbonate-polyorganosiloxane copolymer having high transparency wasobtained. The results of the evaluations of the resultantpolycarbonate-polyorganosiloxane copolymer are shown in Table 2.

Example 7

The transparency of a raw material mixture after its heating treatmentwas evaluated in the same manner as in Example 3 except that 105.4 g ofthe PDMS-1 was used as a polyorganosiloxane. The liquid raw materialmixture after the heating treatment had high transparency, and had atotal light transmittance of 97.5% and a haze value of 0.9.

Polymerization was performed under the same conditions as those ofExample 3 except that 105.4 g of the PDMS-1 was used as apolyorganosiloxane. Thus, a pellet-shapedpolycarbonate-polyorganosiloxane copolymer having high transparency wasobtained. The results of the evaluations of the resultantpolycarbonate-polyorganosiloxane copolymer are shown in Table 2.

Example 8

The transparency of a raw material mixture after its heating treatmentwas evaluated in the same manner as in Example 3 except that 222.5 g ofthe PDMS-1 was used as a polyorganosiloxane. The liquid raw materialmixture after the heating treatment had high transparency, and had atotal light transmittance of 97.1% and a haze value of 1.1.

Polymerization was performed under the same conditions as those ofExample 3 except that 222.5 g of the PDMS-1 was used as apolyorganosiloxane. Thus, a pellet-shapedpolycarbonate-polyorganosiloxane copolymer having high transparency wasobtained. The results of the evaluations of the resultantpolycarbonate-polyorganosiloxane copolymer are shown in Table 2.

Example 9

The transparency of a raw material mixture after its heating treatmentwas evaluated in the same manner as in Example 3 except that ISB(1,193.8 g) and TCDDM (687.2 g) serving as diol monomers, and DPC (2,500g) (molar ratio among the respective raw materials:ISB/TCDDM/DPC=70:30:100), and 22.1 g of the polyether-modifiedpolyorganosiloxane PDMS-1 were used. The liquid raw material mixtureafter the heating treatment had high transparency, and had a total lighttransmittance of 98.5% and a haze value of 0.4.

Polymerization was performed under the same conditions as those ofExample 3 except that ISB (1,193.8 g) and TCDDM (687.2 g) serving asdiol monomers, and DPC (2,500 g) (molar ratio among the respective rawmaterials: ISB/TCDDM/DPC=70:30:100), and 22.1 g of thepolyether-modified polyorganosiloxane PDMS-1 were used. Thus, apellet-shaped polycarbonate-polyorganosiloxane copolymer having hightransparency was obtained. The results of the evaluations of theresultant polycarbonate-polyorganosiloxane copolymer are shown in Table2.

Example 10

The transparency of a raw material mixture after its heating treatmentwas evaluated in the same manner as in Example 3 except that ISB(1,193.8 g), 1,4-CHDM (420.7 g), and 1,3-PG (44.4 g) serving as diolmonomers, and DPC (2,500 g) (molar ratio among the respective rawmaterials: ISB/1,4-CHDM/1,3-PG/DPC=70:25:5:100), and 19.8 g of thepolyether-modified polyorganosiloxane PDMS-1 were used. The liquid rawmaterial mixture after the heating treatment had high transparency, andhad a total light transmittance of 98.3% and a haze value of 0.4.

Polymerization was performed under the same conditions as those ofExample 3 except that ISB (1,193.8 g), 1,4-CHDM (420.7 g), and 1,3-PG(44.4 g) serving as diol monomers, and DPC (2,500 g) (molar ratio amongthe respective raw materials: ISB/1,4-CHDM/1,3-PG/DPC=70:25:5:100), and19.8 g of the polyether-modified polyorganosiloxane PDMS-1 were used.Thus, a pellet-shaped polycarbonate-polyorganosiloxane copolymer havinghigh transparency was obtained. The results of the evaluations of theresultant polycarbonate-polyorganosiloxane copolymer are shown in Table2.

Example 11

The transparency of a raw material mixture after its heating treatmentwas evaluated in the same manner as in Example 3 except that ISB(1,193.8 g), 1,4-CHDM (504.9 g), and PEG 400 (93.4 g) serving as diolmonomers, and DPC (2,500 g) [molar ratio among the respective rawmaterials: ISB/1,4-CHDM/PEG 400/DPC=70:28:2:100 (a value obtained bydividing the used mass of the PEG 400 by its average molecular weight,that is, 400 was used as the number of moles thereof)], and 21.3 g ofthe polyether-modified polyorganosiloxane PDMS-1 were used. The liquidraw material mixture after the heating treatment had high transparency,and had a total light transmittance of 98.3% and a haze value of 0.4.

Polymerization was performed under the same conditions as those ofExample 3 except that ISB (1,193.8 g), 1,4-CHDM (504.9 g), and PEG 400(93.4 g) serving as diol monomers, and DPC (2,500 g) [molar ratio amongthe respective raw materials: ISB/1,4-CHDM/PEG 400/DPC=70:28:2:100 (avalue obtained by dividing the used mass of the PEG 400 by its averagemolecular weight, that is, 400 was used as the number of molesthereof)], and 21.3 g of the polyether-modified polyorganosiloxanePDMS-1 were used. Thus, a pellet-shaped polycarbonate-polyorganosiloxanecopolymer having high transparency was obtained. The results of theevaluations of the resultant polycarbonate-polyorganosiloxane copolymerare shown in Table 2.

Example 12

<Evaluation of Transparency of Raw Material Mixture after its HeatingTreatment>

The transparency of a raw material mixture after its heating treatmentwas evaluated in the same manner as in Example 1 except that 179.7 g ofthe PDMS-8 was used as a polyorganosiloxane. The liquid raw materialmixture after the heating treatment had high transparency, and had atotal light transmittance of 90.8% and a haze value of 2.5.

<Production of PC-POS Copolymer>

Polymerization was performed under the same conditions as those ofExample 1 except that 179.7 g of the PDMS-8 was used as apolyorganosiloxane. Thus, a pellet-shapedpolycarbonate-polyorganosiloxane copolymer having high transparency wasobtained. The resultant polycarbonate-polyorganosiloxane copolymer had aviscosity-average molecular weight of 20,100, a polydimethylsiloxanecontent of 5.00 mass %, a total light transmittance of 33.7%, a hazevalue of 97.0, and a Charpy impact strength (with a notch) of 81.0kJ/m².

Example 13

<Evaluation of Transparency of Raw Material Mixture after its HeatingTreatment>

The transparency of a raw material mixture after its heating treatmentwas evaluated in the same manner as in Example 1 except that 312.8 g ofthe PDMS-8 was used as a polyorganosiloxane. The liquid raw materialmixture after the heating treatment had high transparency, and had atotal light transmittance of 89.1% and a haze value of 2.6.

<Production of PC-POS Copolymer>

Polymerization was performed under the same conditions as those ofExample 1 except that 312.8 g of the PDMS-8 was used as apolyorganosiloxane. Thus, a pellet-shapedpolycarbonate-polyorganosiloxane copolymer having high transparency wasobtained. The resultant polycarbonate-polyorganosiloxane copolymer had aviscosity-average molecular weight of 20,100, a polydimethylsiloxanecontent of 8.30 mass %, a total light transmittance of 28.3%, a hazevalue of 98.1, and a Charpy impact strength (with a notch) of 85.0kJ/m².

Example 14

<Evaluation of Transparency of Raw Material Mixture after its HeatingTreatment>

The transparency of a raw material mixture after its heating treatmentwas evaluated in the same manner as in Example 1 except that 179.7 g ofthe PDMS-9 was used as a polyorganosiloxane. The liquid raw materialmixture after the heating treatment had high transparency, and had atotal light transmittance of 90.1% and a haze value of 2.0.

<Production of PC-POS Copolymer>

Polymerization was performed under the same conditions as those ofExample 1 except that 179.7 g of the PDMS-9 was used as apolyorganosiloxane. Thus, a pellet-shapedpolycarbonate-polyorganosiloxane copolymer having high transparency wasobtained. The resultant polycarbonate-polyorganosiloxane copolymer had aviscosity-average molecular weight of 20,000, a polydimethylsiloxanecontent of 3.10 mass %, a total light transmittance of 62.0%, a hazevalue of 89.4, and a Charpy impact strength (with a notch) of 75.0kJ/m².

Example 15

<Evaluation of Transparency of Raw Material Mixture after its HeatingTreatment>

The transparency of a raw material mixture after its heating treatmentwas evaluated in the same manner as in Example 1 except that 179.7 g ofthe PDMS-10 was used as a polyorganosiloxane. The liquid raw materialmixture after the heating treatment had high transparency, and had atotal light transmittance of 91.0% and a haze value of 1.3.

<Production of PC-POS Copolymer>

Polymerization was performed under the same conditions as those ofExample 1 except that 179.7 g of the PDMS-10 was used as apolyorganosiloxane. Thus, a pellet-shapedpolycarbonate-polyorganosiloxane copolymer having high transparency wasobtained. The resultant polycarbonate-polyorganosiloxane copolymer had aviscosity-average molecular weight of 20,150, a polydimethylsiloxanecontent of 0.90 mass %, a total light transmittance of 86.1%, a hazevalue of 6.8, and a Charpy impact strength (with a notch) of 76.0 kJ/m².

Example 16

<Evaluation of Transparency of Raw Material Mixture after its HeatingTreatment>

The transparency of a raw material mixture after its heating treatmentwas evaluated in the same manner as in Example 1 except that 28.2 g ofthe PDMS-11 was used as a polyorganosiloxane. The liquid raw materialmixture after the heating treatment had high transparency, and had atotal light transmittance of 89.9% and a haze value of 7.3.

<Production of PC-POS Copolymer>

Polymerization was performed under the same conditions as those ofExample 1 except that 28.2 g of the PDMS-11 was used as apolyorganosiloxane. Thus, a pellet-shapedpolycarbonate-polyorganosiloxane copolymer having high transparency wasobtained. The resultant polycarbonate-polyorganosiloxane copolymer had aviscosity-average molecular weight of 20,200, a polydimethylsiloxanecontent of 0.53 mass %, a total light transmittance of 65.1%, and a hazevalue of 83.5.

Example 17

<Evaluation of Transparency of Raw Material Mixture after its HeatingTreatment>

The transparency of a raw material mixture after its heating treatmentwas evaluated in the same manner as in Example 1 except that 57.1 g ofthe PDMS-11 was used as a polyorganosiloxane. The liquid raw materialmixture after the heating treatment had high transparency, and had atotal light transmittance of 78.6% and a haze value of 12.0.

<Production of PC-POS Copolymer>

Polymerization was performed under the same conditions as those ofExample 1 except that 57.1 g of the PDMS-11 was used as apolyorganosiloxane. Thus, a pellet-shapedpolycarbonate-polyorganosiloxane copolymer having high transparency wasobtained. The resultant polycarbonate-polyorganosiloxane copolymer had aviscosity-average molecular weight of 20,100, a polydimethylsiloxanecontent of 1.10 mass %, a total light transmittance of 48.1%, and a hazevalue of 87.5.

Example 18

<Evaluation of Transparency of Raw Material Mixture after its HeatingTreatment>

The transparency of a raw material mixture after its heating treatmentwas evaluated in the same manner as in Example 1 except that 28.2 g ofthe PDMS-12 was used as a polyorganosiloxane. The liquid raw materialmixture after the heating treatment had high transparency, and had atotal light transmittance of 97.9% and a haze value of 0.9.

<Production of PC-POS Copolymer>

Polymerization was performed under the same conditions as those ofExample 1 except that 28.2 g of the PDMS-12 was used as apolyorganosiloxane. Thus, a pellet-shapedpolycarbonate-polyorganosiloxane copolymer having high transparency wasobtained. The resultant polycarbonate-polyorganosiloxane copolymer had aviscosity-average molecular weight of 19,900, a polydimethylsiloxanecontent of 0.45 mass %, a total light transmittance of 81.0%, and a hazevalue of 11.3.

Example 19

<Evaluation of Transparency of Raw Material Mixture after its HeatingTreatment>

The transparency of a raw material mixture after its heating treatmentwas evaluated in the same manner as in Example 1 except that 179.7 g ofthe PDMS-12 was used as a polyorganosiloxane. The liquid raw materialmixture after the heating treatment had high transparency, and had atotal light transmittance of 91.3% and a haze value of 2.1.

<Production of PC-POS Copolymer>

Polymerization was performed under the same conditions as those ofExample 1 except that 179.7 g of the PDMS-12 was used as apolyorganosiloxane. Thus, a pellet-shapedpolycarbonate-polyorganosiloxane copolymer having high transparency wasobtained. The resultant polycarbonate-polyorganosiloxane copolymer had aviscosity-average molecular weight of 20,100, a polydimethylsiloxanecontent of 2.70 mass %, a total light transmittance of 61.0%, and a hazevalue of 82.1.

Example 20

<Evaluation of Transparency of Raw Material Mixture after its HeatingTreatment>

The transparency of a raw material mixture after its heating treatmentwas evaluated in the same manner as in Example 1 except that 28.2 g ofthe PDMS-13 was used as a polyorganosiloxane. The liquid raw materialmixture after the heating treatment had high transparency, and had atotal light transmittance of 91.5% and a haze value of 8.5.

<Production of PC-POS Copolymer>

Polymerization was performed under the same conditions as those ofExample 1 except that 28.2 g of the PDMS-13 was used as apolyorganosiloxane. Thus, a pellet-shapedpolycarbonate-polyorganosiloxane copolymer having high transparency wasobtained. The resultant polycarbonate-polyorganosiloxane copolymer had aviscosity-average molecular weight of 20,050, a polydimethylsiloxanecontent of 0.42 mass %, a total light transmittance of 63.5%, and a hazevalue of 81.2.

Example 21

<Evaluation of Transparency of Raw Material Mixture after its HeatingTreatment>

The transparency of a raw material mixture after its heating treatmentwas evaluated in the same manner as in Example 3 except that 20.2 g ofthe PDMS-14 was used as a polyorganosiloxane. The liquid raw materialmixture after the heating treatment had high transparency, and had atotal light transmittance of 98.1% and a haze value of 1.0.

<Production of PC-POS Copolymer>

Polymerization was performed under the same conditions as those ofExample 2 except that 20.2 g of the PDMS-14 was used as apolyorganosiloxane. Thus, a pellet-shapedpolycarbonate-polyorganosiloxane copolymer having high transparency wasobtained. The resultant polycarbonate-polyorganosiloxane copolymer had aviscosity-average molecular weight of 15,000, a polydimethylsiloxanecontent of 0.68 mass %, a total light transmittance of 69.7%, and a hazevalue of 84.0.

Comparative Example 1

The transparency of a raw material mixture after its heating treatmentwas evaluated in the same manner as in Example 1 except that 28.2 g ofthe PDMS-5 was used as a polyorganosiloxane. The liquid raw materialmixture after the heating treatment was cloudy, and had a total lighttransmittance of 77.6% and a haze value of 95.4.

Polymerization was performed under the same conditions as those ofExample 1 except that 28.2 g of the PDMS-5 was used as apolyorganosiloxane. Thus, a pellet-shapedpolycarbonate-polyorganosiloxane copolymer that was strongly cloudy wasobtained. The results of the evaluations of the resultantpolycarbonate-polyorganosiloxane copolymer are shown in Table 3.

Comparative Example 2

The transparency of a raw material mixture after its heating treatmentwas evaluated in the same manner as in Example 2 except that 24.4 g ofthe PDMS-5 was used as a polyorganosiloxane. The liquid raw materialmixture after the heating treatment was cloudy, and had a total lighttransmittance of 78.5% and a haze value of 93.2.

Polymerization was performed under the same conditions as those ofExample 2 except that 24.4 g of the PDMS-5 was used as apolyorganosiloxane. Thus, a pellet-shapedpolycarbonate-polyorganosiloxane copolymer that was strongly cloudy wasobtained. The results of the evaluations of the resultantpolycarbonate-polyorganosiloxane copolymer are shown in Table 3.

Comparative Example 3

The transparency of a raw material mixture after its heating treatmentwas evaluated in the same manner as in Example 3 except that 20.2 g ofthe PDMS-5 was used as a polyorganosiloxane. The liquid raw materialmixture after the heating treatment was cloudy, and had a total lighttransmittance of 79.1% and a haze value of 92.1.

Polymerization was performed under the same conditions as those ofExample 3 except that 20.2 g of the PDMS-5 was used as apolyorganosiloxane. Thus, a pellet-shapedpolycarbonate-polyorganosiloxane copolymer that was strongly cloudy wasobtained. The results of the evaluations of the resultantpolycarbonate-polyorganosiloxane copolymer are shown in Table 3.

Comparative Example 4

The transparency of a raw material mixture after its heating treatmentwas evaluated in the same manner as in Example 3 except that 105.4 g ofthe PDMS-5 was used as a polyorganosiloxane. The liquid raw materialmixture after the heating treatment was cloudy, and had a total lighttransmittance of 63.2% and a haze value of 95.5.

Polymerization was performed under the same conditions as those ofExample 3 except that 105.4 g of the PDMS-5 was used as apolyorganosiloxane. Thus, a pellet-shapedpolycarbonate-polyorganosiloxane copolymer that was strongly cloudy wasobtained. The results of the evaluations of the resultantpolycarbonate-polyorganosiloxane copolymer are shown in Table 3.

Comparative Example 5

The transparency of a raw material mixture after its heating treatmentwas evaluated in the same manner as in Example 3 except that 20.2 g ofthe PDMS-6 was used as a polyorganosiloxane. The liquid raw materialmixture after the heating treatment was cloudy, and had a total lighttransmittance of 79.5% and a haze value of 93.1.

Polymerization was performed under the same conditions as those ofExample 3 except that 20.2 g of the PDMS-6 was used as apolyorganosiloxane. Thus, a pellet-shapedpolycarbonate-polyorganosiloxane copolymer that was strongly cloudy wasobtained. The results of the evaluations of the resultantpolycarbonate-polyorganosiloxane copolymer are shown in Table 3.

Comparative Example 6

The transparency of a raw material mixture after its heating treatmentwas evaluated in the same manner as in Example 3 except that 20.2 g ofthe PDMS-7 was used as a polyorganosiloxane. The liquid raw materialmixture after the heating treatment was cloudy, and had a total lighttransmittance of 81.1% and a haze value of 88.9.

Polymerization was performed under the same conditions as those ofExample 3 except that 20.2 g of the PDMS-7 was used as apolyorganosiloxane. Thus, a pellet-shapedpolycarbonate-polyorganosiloxane copolymer that was strongly cloudy wasobtained. The results of the evaluations of the resultantpolycarbonate-polyorganosiloxane copolymer are shown in Table 3.

Comparative Example 7

The transparency of a raw material mixture after its heating treatmentwas evaluated in the same manner as in Example 9 except that 22.1 g ofthe PDMS-5 was used as a polyorganosiloxane. The liquid raw materialmixture after the heating treatment was cloudy, and had a total lighttransmittance of 80.1% and a haze value of 90.1.

Polymerization was performed under the same conditions as those ofExample 9 except that 22.1 g of the PDMS-5 was used as apolyorganosiloxane. Thus, a pellet-shapedpolycarbonate-polyorganosiloxane copolymer that was strongly cloudy wasobtained. The results of the evaluations of the resultantpolycarbonate-polyorganosiloxane copolymer are shown in Table 3.

Comparative Example 8

The transparency of a raw material mixture after its heating treatmentwas evaluated in the same manner as in Example 10 except that 19.8 g ofthe PDMS-5 was used as a polyorganosiloxane. The liquid raw materialmixture after the heating treatment was cloudy, and had a total lighttransmittance of 78.5% and a haze value of 89.9.

Polymerization was performed under the same conditions as those ofExample 10 except that 19.8 g of the PDMS-5 was used as apolyorganosiloxane. Thus, a pellet-shapedpolycarbonate-polyorganosiloxane copolymer that was strongly cloudy wasobtained. The results of the evaluations of the resultantpolycarbonate-polyorganosiloxane copolymer are shown in Table 3.

Comparative Example 9

The transparency of a raw material mixture after its heating treatmentwas evaluated in the same manner as in Example 11 except that 21.3 g ofthe PDMS-5 was used as a polyorganosiloxane. The liquid raw materialmixture after the heating treatment was cloudy, and had a total lighttransmittance of 79.9% and a haze value of 88.5.

Polymerization was performed under the same conditions as those ofExample 11 except that 21.3 g of the PDMS-5 was used as apolyorganosiloxane. Thus, a pellet-shapedpolycarbonate-polyorganosiloxane copolymer that was strongly cloudy wasobtained. The results of the evaluations of the resultantpolycarbonate-polyorganosiloxane copolymer are shown in Table 3.

Comparative Example 10

The transparency of a raw material mixture after its heating treatmentwas evaluated in the same manner as in Example 1 except that 179.7 g ofthe PDMS-5 was used as a polyorganosiloxane. The liquid raw materialmixture after the heating treatment was cloudy, and had a total lighttransmittance of 65.1% and a haze value of 97.5.

Polymerization was performed under the same conditions as those ofExample 1 except that 179.7 g of the PDMS-5 was used as apolyorganosiloxane. Thus, a pellet-shapedpolycarbonate-polyorganosiloxane copolymer that was strongly cloudy wasobtained. The resultant polycarbonate-polyorganosiloxane copolymer had aviscosity-average molecular weight of 20,000, a polydimethylsiloxanecontent of 5.30 mass %, a total light transmittance of 19.3%, a hazevalue of 99.6, and a Charpy impact strength (with a notch) of 61.0kJ/m².

Comparative Example 11

The transparency of a raw material mixture after its heating treatmentwas evaluated in the same manner as in Example 1 except that 179.7 g ofthe PDMS-7 was used as a polyorganosiloxane. The liquid raw materialmixture after the heating treatment was cloudy, and had a total lighttransmittance of 66.5% and a haze value of 96.2.

Polymerization was performed under the same conditions as those ofExample 1 except that 179.7 g of the PDMS-7 was used as apolyorganosiloxane. Thus, a pellet-shapedpolycarbonate-polyorganosiloxane copolymer that was strongly cloudy wasobtained. The resultant polycarbonate-polyorganosiloxane copolymer had aviscosity-average molecular weight of 20,100, a polydimethylsiloxanecontent of 5.50 mass %, a total light transmittance of 17.5%, a hazevalue of 99.5, and a Charpy impact strength (with a notch) of 61.0kJ/m².

TABLE 2 Example Unit 1 2 3 4 5 6 Loading Diol monomer BisP-A Molar 10050 condition (A) ISB ratio 70 70 70 70 1,4-CHDM 50 30 30 30 30 TCDDM1,3-PG PEG 400 Carbonic acid DPC 107 103 100 100 100 100 diesterPolyorgano- PDMS-1 wt %* 1 1 1 siloxane (B) PDMS-2 1 PDMS-3 1 PDMS-4 1PDMS-5 PDMS-6 PDMS-7 Evaluation Raw material Total light % 98.4 98.599.5 98.4 98.1 97.9 result mixture after its transmittance heatingtreatment Haze value — 0.5 0.5 0.4 0.8 1.3 0.7 PC-POS Polyorgano- wt %0.62 0.63 0.62 0.73 0.82 0.67 copolymer siloxane represented by formula(1) Viscosity-average Mv 15,500 15,100 14,900 15,100 15,100 14,500molecular weight Total light trans- % 82.0 84.0 91.1 86.5 80.1 90.2mittance (1 mmt) Haze value — 5.5 4.1 0.7 3.1 5.8 1.3 Charpy impactkJ/m² 20.3 22.4 9.8 10.8 12.1 8.7 strength (with a notch) Example Unit 78 9 10 11 Loading Diol monomer BisP-A Molar condition (A) ISB ratio 7070 70 70 70 1,4-CHDM 30 30 25 28 TCDDM 30 1,3-PG 5 PEG 400 2 Carbonicacid DPC 100 100 100 100 100 diester Polyorgano- PDMS-1 wt %* 5 10 1 1 1siloxane (B) PDMS-2 PDMS-3 PDMS-4 PDMS-5 PDMS-6 PDMS-7 Evaluation Rawmaterial Total light % 97.5 97.1 98.5 98.3 98.3 result mixture after itstransmittance heating treatment Haze value — 0.9 1.1 0.4 0.4 0.4 PC-POSPolyorgano- wt % 3.3 6.3 0.61 0.62 0.62 copolymer siloxane representedby formula (1) Viscosity-average Mv 15,400 15,300 15,100 14,800 14,900molecular weight Total light trans- % 90.5 88.9 90.8 91.2 90.9 mittance(1 mmt) Haze value — 1.9 3.6 0.7 0.9 0.9 Charpy impact kJ/m² 12.5 14.58.9 10.5 10.8 strength (with a notch) *The wt % of thepolyorganosiloxane (B) represents the amount of the loadedpolyorganosiloxane (B) in the mass (theoretical value of the PC-POScopolymer to be obtained. The numerical value was determined from thefollowing equation. Mass (theoretical value) of PC-POS copolymer = massof all diol monomers + mass of carbonic acid diester + mass ofpolyorganosiloxane (B) − mass of produced phenol (phenol whose molaramount is twice as large as that of the carbonic acid diester)

TABLE 3 Comparative Example Unit 1 2 3 4 5 Loading Diol monomer BisP-AMolar 100 50 condition (A) ISB ratio 70 70 70 1,4-CHDM 50 30 30 30 TCDDM1,3-PG PEG 400 Carbonic acid DPC 107 103 100 100 100 diester Polyorgano-PDMS-1 wt %* siloxane (B) PDMS-2 PDMS-3 PDMS-4 PDMS-5 1 1 1 5 PDMS-6 1PDMS-7 Evaluation Raw material Total light % 77.6 78.5 79.1 63.2 79.5result mixture after its transmittance heating treatment Haze value —95.4 93.2 92.1 95.5 93.1 PC-POS Polyorgano- wt % 0.87 0.87 0.88 4.010.87 copolymer siloxane represented by formula (1) Viscosity-average Mv15,000 15,100 15,300 15,100 15,300 molecular weight Total light trans- %49.6 51.1 52.7 41.0 51.25 mittance (1 mmt) Haze value — 99.6 99.3 99.699.8 98.2 Charpy impact kJ/m² 15.4 14.2 6.1 6.8 6.2 strength (with anotch) Comparative Example Unit 6 7 8 9 Loading Diol monomer BisP-AMolar condition (A) ISB ratio 70 70 70 70 1,4-CHDM 30 25 28 TCDDM 30 301,3-PG 5 PEG 400 2 Carbonic acid DPC 100 100 100 100 diester Polyorgano-PDMS-1 wt %* siloxane (B) PDMS-2 PDMS-3 PDMS-4 PDMS-5 1 1 1 PDMS-6PDMS-7 1 Evaluation Raw material Total light % 81.1 80.1 78.52 79.9result mixture after its transmittance heating treatment Haze value —88.9 90.1 89.9 88.5 PC-POS Polyorgano- wt % 0.89 0.86 0.87 0.88copolymer siloxane represented by formula (1) Viscosity-average Mv14,900 14,900 15,100 15,000 molecular weight Total light trans- % 50.151.6 49.9 53.1 mittance (1 mmt) Haze value — 98.5 99.2 98.2 97.5 Charpyimpact kJ/m² 6.0 6.3 6.3 6.4 strength (with a notch) *The wt % of thepolyorganosiloxane (B) represents the amount of the loadedpolyorganosiloxane (B) in the mass (theoretical value of the PC-POScopolymer to be obtained. The numerical value was determined from thefollowing equation. Mass (theoretical value) of PC-POS copolymer = massof all diol monomers + mass of carbonic acid diester + mass ofpolyorganosiloxane (B) − mass of produced phenol (phenol whose molaramount is twice as large as that of the carbonic acid diester)

1. A polycarbonate-polyorganosiloxane copolymer, which is produced byusing a diol monomer (a1) and a polyorganosiloxane (a2) satisfying thefollowing condition, comprising: a polyorganosiloxane block (A-1)including a repeating unit represented by the following formula (1); anda polycarbonate block (A-2) formed of a repeating unit represented bythe following formula (2): a mixture, which is obtained by bringing thediol monomer (a1), the polyorganosiloxane (a2), a carbonic acid diester,and a basic catalyst present at the same amount ratio as that at a timeof production of the polycarbonate-polyorganosiloxane copolymer intocontact with each other at from 100° C. to 250° C. for from 0.5 hour to5 hours, has a haze value of 30 or less measured under conditions of 23°C. and an optical path length of 10 mm in conformity with ISO14782:1999:

wherein R¹ and R² may be identical to or different from each other, andeach independently represent a hydrogen atom, a halogen atom, an alkylgroup having 1 to 10 carbon atoms, an alkoxy group having 1 to 10 carbonatoms, an aryl group having 6 to 12 carbon atoms, or an alkylaryl groupwhose alkyl group moiety has 1 to 10 carbon atoms, “a” represents aninteger of from 2 to 500, R¹⁰ represents a divalent aliphatichydrocarbon group having 2 to 40 carbon atoms or a divalent alicyclichydrocarbon group having 3 to 40 carbon atoms, or a divalent aromatichydrocarbon group having 6 to 20 carbon atoms, and may be substitutedwith a substituent, the divalent aliphatic hydrocarbon group, thedivalent alicyclic hydrocarbon group, or the divalent aromatichydrocarbon group may contain at least one heteroatom selected from anoxygen atom, a nitrogen atom, and a sulfur atom, or at least one halogenatom selected from a fluorine atom, a chlorine atom, a bromine atom, andan iodine atom, and “y” represents an integer of from 10 to
 500. 2. Thepolycarbonate-polyorganosiloxane copolymer according to claim 1, furthercomprising a structural unit represented by the following formula (3):

wherein R³ and R⁴ may be identical to or different from each other, andeach independently represent a hydrogen atom, a halogen atom, an alkylgroup having 1 to 10 carbon atoms, an alkoxy group having 1 to 10 carbonatoms, an aryl group having 6 to 12 carbon atoms, or an alkylaryl groupwhose alkyl group moiety has 1 to 10 carbon atoms, R⁶ represents anarylene group having 6 to 20 carbon atoms, an alkylene group having 1 to10 carbon atoms, or an alkylarylene group whose alkyl group moiety has 1to 10 carbon atoms, and may contain, as a functional group, —O—, —COO—,—CO—, —S—, —NH—, or —NR¹¹¹—, R⁸s may be identical to or different fromeach other, and each independently represent an arylene group having 6to 20 carbon atoms, an alkylene group having 1 to 10 carbon atoms, abranched alkylene group having 3 to 10 carbon atoms, or an alkylarylenegroup whose alkyl group moiety has 1 to 10 carbon atoms, and may eachcontain, as a functional group, —O—, —COO—, —CO—, —S—, —NH—, or —NR¹¹¹—,R¹¹¹ represents an alkyl group having 1 to 10 carbon atoms or an arylgroup having 6 to 10 carbon atoms, “z” represents 0 or 1, and “b”represents an integer of from 0 to
 200. 3. Thepolycarbonate-polyorganosiloxane copolymer according to claim 1, whereinthe polyorganosiloxane block (A-1) includes a structure represented bythe following formula (I):

wherein R¹ to R⁴ may be identical to or different from each other, andeach independently represent a hydrogen atom, a halogen atom, an alkylgroup having 1 to 10 carbon atoms, an alkoxy group having 1 to 10 carbonatoms, an aryl group having 6 to 12 carbon atoms, or an alkylaryl groupwhose alkyl group moiety has 1 to 10 carbon atoms, R⁵ and R⁶ may beidentical to or different from each other, and each independentlyrepresent an arylene group having 6 to 20 carbon atoms, an alkylenegroup having 1 to 10 carbon atoms, or an alkylarylene group whose alkylgroup moiety has 1 to 10 carbon atoms, and may each contain, as afunctional group, —O—, —COO—, —CO—, —S—, —NH—, or —NR¹¹¹—, R⁷ and R⁸ maybe identical to or different from each other, and each independentlyrepresent an arylene group having 6 to 20 carbon atoms, an alkylenegroup having 1 to 10 carbon atoms, a branched alkylene group having 3 to10 carbon atoms, or an alkylarylene group whose alkyl group moiety has 1to 10 carbon atoms, and may each contain, as a functional group, —O—,—COO—, —CO—, —S—, —NH—, or —NR¹¹¹—, R¹¹¹ represents an alkyl grouphaving 1 to 10 carbon atoms or an aryl group having 6 to 10 carbonatoms, “z” and “z1” each independently represent 0 or 1, “a” representsan integer of from 2 to 500, and “b” and “b1” each independentlyrepresent an integer of from 0 to
 200. 4. Thepolycarbonate-polyorganosiloxane copolymer according to claim 1, whereinthe diol monomer (a1) is at least one kind of compound selected from thegroup consisting of an aromatic dihydroxy compound represented by thefollowing formula (111) and an aliphatic dihydroxy compound representedby the following formula (112):

wherein R⁵⁵ and R⁵⁶ each independently represent a halogen atom, analkyl group having 1 to 6 carbon atoms, or an alkoxy group having 1 to 6carbon atoms, X represents a single bond, an alkylene group having 1 to8 carbon atoms, an alkylidene group having 2 to 8 carbon atoms, acycloalkylene group having 5 to 15 carbon atoms, a cycloalkylidene grouphaving 5 to 15 carbon atoms, a fluorenediyl group, an arylalkylene grouphaving 7 to 15 carbon atoms, an arylalkylidene group having 7 to 15carbon atoms, —S—, —SO—, —SO₂—, —O—, or —CO—, “s” and “t” eachindependently represent an integer of from 0 to 4, R¹⁰⁰ represents adivalent aliphatic hydrocarbon group having 2 to 40 carbon atoms, andmay include a branched structure or a cyclic structure, and R¹⁰⁰ maycontain at least one heteroatom selected from an oxygen atom, a nitrogenatom, and a sulfur atom, or at least one halogen atom selected from afluorine atom, a chlorine atom, a bromine atom, and an iodine atom. 5.The polycarbonate-polyorganosiloxane copolymer according to claim 1,wherein the diol monomer (a1) is an aromatic bisphenol selected from2,2-bis(4-hydroxyphenyl)propane,2,2-bis(4-hydroxy-3-methylphenyl)propane,1,1-bis(4-hydroxyphenyl)cyclohexane,1,1-bis(4-hydroxyphenyl)-3-methylcyclohexane,1,1-bis(4-hydroxyphenyl)-3,3,5-trimethylcyclohexane, and1,1-bis(4-hydroxyphenyl)cyclododecene, or an aliphatic diol selectedfrom isosorbide, cyclohexane-1,4-dimethanol, tricyclodecanedimethanol,3,9-bis(1,1-dimethyl-2-hydroxyethyl)-2,4,8,10-tetraoxaspiro[5.5]undecane,1,3-propanediol, and 1,4-butanediol.
 6. Thepolycarbonate-polyorganosiloxane copolymer according to claim 1, whereinthe polycarbonate block (A-2) includes one or more selected from thegroup consisting of repeating units represented by the followingformulae (a-i) to (a-v):


7. The polycarbonate-polyorganosiloxane copolymer according to claim 1,wherein in the formula (1) or the formula (I), “a” represents an integerof 2 or more and 300 or less.
 8. The polycarbonate-polyorganosiloxanecopolymer according to claim 1, wherein the polyorganosiloxane block(A-1) includes at least one selected from the group consisting ofstructural units represented by the following formulae (1-1) to (1-3):

wherein 10 to R⁸, “z”, “z1”, “a”, “b”, and “b1” are as described above,and β represents a divalent group derived from a diisocyanate compound,or a divalent group derived from a dicarboxylic acid or a dicarboxylicacid halide.
 9. The polycarbonate-polyorganosiloxane copolymer accordingto claim 1, wherein R¹ and R² in the formula (1), or R¹ to R⁴ in theformula (1) and the formula (3) each represent a methyl group.
 10. Thepolycarbonate-polyorganosiloxane copolymer according to claim 2, whereinin the formula (3), R⁶ represents a trimethylene group (—(CH₂)₃—). 11.The polycarbonate-polyorganosiloxane copolymer according to claim 2,wherein in the formula (3), R⁸ represents any structure selected fromthe group consisting of a dimethylene group (—(CH₂)₂—), amethyl-substituted dimethylene group (—CH₂CHMe—), a trimethylene group(—(CH₂)₃—), and a tetramethylene group (—(CH₂)₄—).
 12. Thepolycarbonate-polyorganosiloxane copolymer according to claim 1, whereina content of the polyorganosiloxane block represented by the formula (1)or the formula (I) in the polycarbonate-polyorganosiloxane copolymer is0.1 mass % or more and 60 mass % or less.
 13. Thepolycarbonate-polyorganosiloxane copolymer according to claim 1, whereinthe polycarbonate-polyorganosiloxane copolymer has a viscosity-averagemolecular weight (Mv) of 5,000 or more and 50,000 or less.
 14. Thepolycarbonate-polyorganosiloxane copolymer according to claim 1, whereina 1-millimeter thick plate obtained by molding thepolycarbonate-polyorganosiloxane copolymer has a haze value of 40 orless measured in conformity with ISO 14782:1999.
 15. Thepolycarbonate-polyorganosiloxane copolymer according to claim 1, whereinthe polycarbonate-polyorganosiloxane copolymer is obtained by a meltpolymerization method.
 16. The polycarbonate-polyorganosiloxanecopolymer according to claim 1, wherein the carbonic acid diester is atleast one kind of compound selected from a diaryl carbonate compound, adialkyl carbonate compound, and an alkyl aryl carbonate compound. 17.The polycarbonate-polyorganosiloxane copolymer according to claim 1,wherein the basic catalyst is at least one kind selected from the groupconsisting of an alkali metal compound, an alkaline earth metalcompound, a nitrogen-containing compound, a quaternary phosphonium saltcontaining an aryl group, and a metal compound.
 18. Apolycarbonate-based resin composition, comprising thepolycarbonate-polyorganosiloxane copolymer of claim
 1. 19. Thepolycarbonate-based resin composition according to claim 18, furthercomprising an inorganic filler.
 20. The polycarbonate-based resincomposition according to claim 19, wherein the polycarbonate-based resincomposition comprises 1 part by mass to 150 parts by mass of theinorganic filler with respect to 100 parts by mass of thepolycarbonate-polyorganosiloxane copolymer.
 21. The polycarbonate-basedresin composition according to claim 19, wherein the inorganic filler isa glass fiber or a carbon fiber.
 22. A molded body, comprising thepolycarbonate-based resin composition of claim 18.